KR20230068831A - Transgenic plant-derived porous carbon material and super capacitor using same - Google Patents
Transgenic plant-derived porous carbon material and super capacitor using same Download PDFInfo
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Abstract
Description
본 발명은 형질전환 식물 유래 다공성 탄소 재료 및 이를 이용한 슈퍼커패시터에 관한 것이다.The present invention relates to a porous carbon material derived from a transgenic plant and a supercapacitor using the same.
전기화학 이중층 커패시터(EDLCs, 슈퍼커패시터로도 지칭됨)는 고전력, 장기간 저장, 및 높은 싸이클 수명을 요구하는 배터리의 대안으로 알려졌다. 전기화학 이중층 커패시터는 고체표면 및 전해질 사이의 경계면에서 전기화학적 이중층에 전기적 전하를 분리 및 저장하여 에너지가 저장된다. Electrochemical double layer capacitors (EDLCs, also referred to as supercapacitors) are known as an alternative to batteries that require high power, long term storage, and high cycle life. In the electrochemical double layer capacitor, energy is stored by separating and storing electric charges in the electrochemical double layer at the interface between the solid surface and the electrolyte.
탄소 나노 물질, 금속 산화물, 전도성 고분자, 및 MXene을 기반으로 한 다양한 슈퍼커패시터 물질이 개발되었다. 그럼에도 불구하고 이러한 재료들은 비용이 높고 지속 가능하지 않은 문제점이 있다. Various supercapacitor materials based on carbon nanomaterials, metal oxides, conductive polymers, and MXene have been developed. Nonetheless, these materials suffer from high cost and unsustainability.
활성 탄소(다공성 탄소 재료)는 매우 넓은 표면적, 우수한 전기적 및 이온 전도도, 우수한 화학적 안전성 및 낮은 가격 덕분에 전기화학 이중층 커패시터로 유망한 물질이다. 활성 탄소는 알칼리 활성화 공정을 거쳐 제작된다. 알칼리 활성화는 KOH 또는 NaOH를 사용한 화학적 활성화로서, 고온의 불활성 대기에서 탄소질의 전구체 화합물을 탄화(carbonization)시킨다. Activated carbon (porous carbon material) is a promising material for electrochemical double layer capacitors thanks to its very large surface area, excellent electrical and ionic conductivity, good chemical stability and low cost. Activated carbon is produced through an alkali activation process. Alkaline activation is a chemical activation using KOH or NaOH, which carbonizes a carbonaceous precursor compound in a high-temperature inert atmosphere.
목재는 지속가능한 소재이며, 슈퍼커패시터 전극에 사용되는 활성 탄소의 원료로서 주목받고 있다. 목질계 바이오매스(lignocellulosic biomass)는 종마다 셀룰로오스, 헤미셀룰로오스, 및 리그난의 함량에 있어서 고유의 화학적 조성을 가지고 있다. 목질계 바이오매스의 화학적 조성과 이들로부터 제작된 다공성 탄소 재료의 에너지 저장 능력은 상호 연관되어 있으나, 그 관계가 명확히 밝혀지지 않은 상태이다. Wood is a sustainable material and is attracting attention as a raw material for activated carbon used in supercapacitor electrodes. Lignocellulosic biomass has a unique chemical composition in terms of cellulose, hemicellulose, and lignan content for each species. Although the chemical composition of lignocellulosic biomass and the energy storage ability of porous carbon materials produced from them are correlated, the relationship has not been clearly identified.
목질계 바이오매스의 화학적 조성이 이로부터 제작된 다공성 탄소 재료의 전기화학적 거동에 미치는 영향을 분석하기 위해서는 동일한 종에서 유래했음에도 화학적 조성이 다른 바이오매스들을 비교해야 한다. 유전 공학의 발전으로 동일한 종에서 유래했음에도 화학 조성이 다른 바이오매스를 제작할 수 있게 됨으로써 목질계 바이오매스의 화학적 조성이 다공성 탄소 재료의 표면 특성 및 전기화학적 거동에 미치는 영향을 조사할 수 있게 되었다.In order to analyze the effect of the chemical composition of lignocellulosic biomass on the electrochemical behavior of the porous carbon material produced therefrom, biomass with different chemical compositions, even though derived from the same species, should be compared. Advances in genetic engineering have made it possible to produce biomass with different chemical compositions even though they are derived from the same species, so that the effect of the chemical composition of lignocellulosic biomass on the surface properties and electrochemical behavior of porous carbon materials can be investigated.
일 구체예는 PdGA20ox1(Pinus densiflora Gibberellin 20-oxidase 1) 유전자 및 PtrMYB221 유전자가 목부조직 특이적으로 발현된 형질전환 식물을 알칼리 활성화 및 탄화시켜 제조한 다공성 탄소 재료 및 이를 이용한 이중층 커패시터 전극을 제공한다.One embodiment provides a porous carbon material prepared by alkaline activation and carbonization of transgenic plants in which the PdGA20ox1 ( Pinus densiflora Gibberellin 20-oxidase 1) gene and the PtrMYB221 gene are specifically expressed in xylem tissue, and a double-layer capacitor electrode using the same.
일 양상은 형질전환 식물로부터 얻은 목질계 바이오매스를 알칼리 활성화 및 탄화시켜 제조한 다공성 탄소 재료로서, 상기 형질전환 식물은 PdGA20ox1(Pinus densiflora Gibberellin 20-oxidase 1) 유전자; 및 PtrMYB221 유전자가 DX15 프로모터에 의해 목부조직 특이적으로 발현된 형질전환 식물인, 다공성 탄소 재료를 제공한다. One aspect is a porous carbon material prepared by alkaline activation and carbonization of woody biomass obtained from transgenic plants, wherein the transgenic plants include a PdGA20ox1 ( Pinus densiflora Gibberellin 20-oxidase 1) gene; and a transgenic plant in which the PtrMYB221 gene is specifically expressed in xylem tissue by the DX15 promoter.
알칼리 활성화 및 탄화는 본 발명의 기술분야에 널리 사용되는 방법을 사용할 수 있다. 일 실시예에 따르면, 상기 알칼리 활성화 및 탄화는 형질전환 식물을 건조 및 분쇄하여 시료를 준비하고, KOH와 혼합하여 질소 기체 하에서 800℃로 탄화시킨 것일 수 있다.Alkaline activation and carbonization can use methods widely used in the art of the present invention. According to one embodiment, the alkali activation and carbonization may be performed by preparing a sample by drying and pulverizing the transgenic plant, mixing it with KOH, and carbonizing it at 800 ° C. under nitrogen gas.
일 구체예에 따르면, 상기 형질전환 식물은 초본 식물 또는 목본 식물일 수 있다. 등록특허 10-1645892에 따르면, 상기 PdGA20ox1 유전자 및 PtrMYB221 유전자가 DX15 프로모터와 작동 가능하게 연결된 벡터로 형질전환된 초본 식물 또는 목본 식물은 상기 유전자가 줄기 또는 목부 특이적으로 발현이 증가함으로써 바이오매스가 증가하고 셀룰로오스 함량이 증가하며 리그닌 함량이 감소하였음을 확인하였다.According to one embodiment, the transgenic plant may be a herbaceous plant or a woody plant. According to Registered Patent No. 10-1645892, herbaceous plants or woody plants in which the PdGA20ox1 gene and the PtrMYB221 gene are transformed with a vector operably linked to the DX15 promoter increase biomass by increasing the expression of the genes specifically in the stem or xylem. It was confirmed that the cellulose content increased and the lignin content decreased.
상기 오리자 사티바(Oryza sativa; 벼), 제아 메이즈(Zea mays; 옥수수), 미스칸투스(Miscanthus) 종, 애기장대풀(Arabidopsis thaliana) 또는 페니세툼 풀푸레움(Pennisetum purpureum) 등일 수 있다.The Oryza sativa (rice), Zea mays (corn), Miscanthus ( Miscanthus ) species, Arabidopsis thaliana or Penisetum purpureum ( Pennisetum purpureum ) and the like.
상기 목본 식물은 유칼립투스(Eucalyptus) 종일 수 있으며, 예를 들면 E. alba, E. albens, E. amygdalina, E. aromaphloia, E. baileyana, E. balladoniensis, E. bicostata, E. botryoides, E. brachyandra, E. brassiana, E. brevistylis, E. brockwayi E. camaldulensis, E. ceracea, E. cloeziana, E. coccifera, E. cordata, E. cornuta, E. corticosa, E. crebra, E. croajingoleisis, E. curtisii, E. dalrympleana, E. deglupta, E. delegatensis, E. delicata, E. diversicolor, E. diversifolia, E. dives, E. dolichocarpa, E. dundasii, E. dunnii, E. elata, E. erythrocoiys, E. erythrophloia, E. eudesmoides, E. falcata, E. gamophylla, E. glaucina, E. globulus, E. globulus subsp. bicostata, E. globulus subsp. globulus, E. gongylocarpa, E. grandis, E. grandisХurophylla, E. guilfoylei, E. gunnii, E. hallii, E. houseana, E. jacksonii, E. lansdowneana, E. latisinensis, E. leucophloia, E. leucoxylon, E. lockyeri, E. lucasii, E. maidenii, E. marginata, E. megacarpa, E. melliodora, E. michaeliana, E. microcorys, E. microtheca, E. muelleriana, E. nitens, E. nitida, E. obliqua, E. obtusiflora, E. occidentalis, E. optima, E. ovata, E. pachyphylla, E. pauciflora, E. pellita, E. perriniana, E. petiolaris, E. pilularis, E. piperita, E. platyphylla, E. polyanthemos, E. populnea, E. preissiana, E. pseudoglobulus, E. pulchella, E. radiata, E. radiata subsp. radiata, E. regnans, E. risdoni, E. robertsonii E. rodwayi, E. rubida, E. rubiginosa, E. saligna, E. salmonophloia, E. scoparia, E. sieberi, E. spathulata, E. staeri E. stoatei, E. tenuipes, E. tenuiramis, E. tereticornis, E. tetragona, E. tetrodonta, E. tindaliae, E. torquata, E. umbra, E. urophylla, E. vernicosa, E. viminalis, E. wandoo, E. wetarensis, E. willisii, E. willisii subsp. falciformis, E. willisii subsp. willisii, E. woodwardii일 수 있다.The woody plant may be a Eucalyptus species, for example, E. alba, E. albens, E. amygdalina, E. aromaphloia, E. baileyana, E. balladoniensis, E. bicostata, E. botryoides, E. brachyandra , E. brassiana, E. brevistylis, E. brockwayi, E. camaldulensis, E. ceracea, E. cloeziana, E. coccifera, E. cordata, E. cornuta, E. corticosa, E. crebra, E. croajingoleisis, E. curtisii, E. dalrympleana, E. deglupta, E. delegatensis, E. delicata, E. diversicolor, E. diversifolia, E. dives, E. dolichocarpa, E. dundasii, E. dunnii, E. elata, E. erythrocoiys, E. erythrophloia, E. eudesmoides, E. falcata, E. gamophylla, E. glaucina, E. globulus, E. globulus subsp. bicostata, E. globulus subsp. globulus, E. gongylocarpa, E. grandis, E. grandisХurophylla, E. guilfoylei, E. gunnii, E. hallii, E. houseana, E. jacksonii, E. lansdowneana, E. latisinensis, E. leucophloia, E. leucoxylon, E. lockyeri, E. lucasii, E. maidenii, E. marginata, E. megacarpa, E. melliodora, E. michaeliana, E. microcorys, E. microtheca, E. muelleriana, E. nitens, E. nitida, E. obliqua, E. obtusiflora, E. occidentalis, E. optima, E. ovata, E. pachyphylla, E. pauciflora, E. pellita, E. perriniana, E. petiolaris, E. pilularis, E. piperita, E. platyphylla, E. polyanthemos, E. populnea, E. preissiana, E. pseudoglobulus, E. pulchella, E. radiata, E. radiata subsp. radiata, E. regnans, E. risdoni, E. robertsonii, E. rodwayi, E. rubida, E. rubiginosa, E. saligna, E. salmonophloia, E. scoparia, E. sieberi, E. spathulata, E. staeri E. stoatei, E. tenuipes, E. tenuiramis, E. tereticornis, E. tetragona, E. tetrodonta, E. tindaliae, E. torquata, E. umbra, E. urophylla, E. vernicosa, E. viminalis, E. wandoo, E. wetarensis, E. willisii, E. willisii subsp. falciformis, E. willisii subsp. willisii, E. woodwardii .
상기 목본 식물은 침엽수(예를 들면, loblolly pine(Pinus taeda), slash pine(Pinus elliotii), ponderosa pine(Pinus ponderosa), lodgepole pine(Pinus contorta), Monterey pine(Pinus radiata); Douglas-fir(Pseudotsuga menziesii); Western hemlock(Tsuga canadensis); Sitka spruce(Picea glauca); redwood(Sequoia sempervirens); silver fir(Abies amabilis); balsam fir(Abies balsamea)), 삼나무(예를 들면 Western red cedar(Thuja plicata), Alaska yellowcedar(Chamecyparis nootkatensis))등일 수 있다.The woody plants are conifers (eg, loblolly pine ( Pinus taeda ), slash pine ( Pinus elliotii ), ponderosa pine ( Pinus ponderosa ), lodgepole pine ( Pinus contorta ), Monterey pine ( Pinus radiata ); Douglas-fir ( Pseudotsuga menziesii ); Western hemlock ( Tsuga canadensis ); Sitka spruce ( Picea glauca ); redwood ( Sequoia sempervirens ); silver fir ( Abies amabilis ); balsam fir ( Abies balsamea )), cedar (e.g. Western red cedar ( Thuja plicata )) , Alaska yellowcedar ( Chamecyparis nootkatensis )) and the like.
상기 목본 식물은 포플러스속(Populus) 식물일 수 있다. 상기 포플러스속 식물은 예를 들면 P. alba, P. albaХP. grandidentata, P. albaХP. tremula, P. albaХP. tremula var. glandulosa, P. albaХP.tremuloides, P. balsamifera, P. balsamifera subsp. trichocarpa, P. balsamifera subsp. trichocarpaХP.deltoides, P. ciliata, P. deltoides, P. euphratica, P. euramericana, P. kitakamiensis, P. lasiocarpa, P. laurifolia, P. maximowiczii, P. maximowicziiХP. balsamfera subsp. trichocarpa, P. nigra, P.sieboldiiХP. grandideiztata, P. suaveolens, P. szechuanica, P. tomentosa, P. tremula, P. tremulaХP. tremuloides, P. tremuloides, P. wilsonii, P. canadensis, P. yunnanensis일 수 있으나 이에 한정되는 것은 아니다.The woody plant may be a Populus genus plant. Plants of the genus Populus are, for example , P. alba, P. albaХP. grandidentata, P. albaХP. tremula, P. albaХP. tremula var. glandulosa, P. albaХP.tremuloides, P. balsamifera, P. balsamifera subsp. trichocarpa, P. balsamifera subsp. trichocarpaХP.deltoides, P. ciliata, P. deltoides, P. euphratica, P. euramericana, P. kitakamiensis, P. lasiocarpa, P. laurifolia, P. maximowiczii, P. maximowicziiХP. balsamfera subsp. trichocarpa, P. nigra, P. sieboldiiХP. grandideiztata, P. suaveolens, P. szechuanica, P. tomentosa, P. tremula, P. tremulaХP. tremuloides, P. tremuloides, P. wilsonii, P. canadensis, P. yunnanensis, but is not limited thereto.
일 구체예에 따르면, 상기 PdGA20ox1 유전자는 서열번호 1의 서열로 이루어진 것이고, 상기 PtrMYB221 유전자는 서열번호 2의 서열로 이루어진 것일 수 있다. According to one embodiment, the PdGA20ox1 gene may consist of the sequence of SEQ ID NO: 1, and the PtrMYB221 gene may consist of the sequence of SEQ ID NO: 2.
상기 DX15 프로모터는 줄기 또는 목부 특이적으로 발현을 유도하는 프로모터로써, 서열번호 3의 서열로 이루어진 것일 수 있다.The DX15 promoter is a promoter that specifically induces expression in the stem or neck, and may be composed of the sequence of SEQ ID NO: 3.
상기 형질전환 식물은 대한민국 등록특허 제10-1645892호에 기재된 방법을 참고하여 제작할 수 있다. 일 실시예에 따르면, pMDC32 벡터의 프로모터를 목부(줄기) 특이적 과발현을 유도하는 DX15 프로모터로 교체하고, DX15-pMDC32 벡터에 PdGA20ox1, PtrMYB221, 또는 이들의 조합을 도입하여 형질전환용 벡터를 제작하고, 제작된 벡터로 아그로박테리움 투메파시엔스(Agrobacterium tumefaciens) 균주 C58을 형질감염(transfection)시키고, 형질전환 균주를 이용하여 식물을 형질전환(transformation)시켜 제작할 수 있다.The transgenic plant can be produced by referring to the method described in Korean Patent Registration No. 10-1645892. According to one embodiment, the promoter of the pMDC32 vector is replaced with the DX15 promoter that induces xylem (stem)-specific overexpression, and PdGA20ox1, PtrMYB221, or a combination thereof is introduced into the DX15-pMDC32 vector to construct a vector for transformation , Agrobacterium tumefaciens ( Agrobacterium tumefaciens ) strain C58 is transfected with the prepared vector, and it can be produced by transforming plants using the transformed strain.
또한 일 실시예에 따르면, PdGA20ox1 및 PtrMYB221 유전자를 목부(줄기) 특이적으로 발현하기 위해 PdGA20ox1 및 PtrMYB221 서열을 2A 펩티드 서열로 연결한 서열을 도입하여 제작한 DX15::PdGA20ox1-2A-PtrMYB221 벡터를 이용할 수 있다. 2A 펩티드 서열은 서열번호 4의 서열로 이루어진 것일 수 있다. In addition, according to one embodiment, a DX15::PdGA20ox1-2A-PtrMYB221 vector prepared by introducing a sequence in which the PdGA20ox1 and PtrMYB221 sequences are linked to a 2A peptide sequence is used to express the PdGA20ox1 and PtrMYB221 genes specifically in the xylem (stem). can The 2A peptide sequence may consist of the sequence of SEQ ID NO: 4.
일 구체예에 따르면, 상기 형질전환 식물은 동종의 야생형 식물보다 셀룰로오스 함량이 증가하고 리그닌의 함량이 감소한 것일 수 있다. According to one embodiment, the transgenic plant may have an increased cellulose content and a reduced lignin content compared to wild-type plants of the same species.
일 구체예에 따르면, 상기 다공성 탄소 재료는 라만 스펙트럼에서 ID/IG의 비율이 동종의 야생형 식물 유래 다공성 탄소 재료보다 낮은 것일 수 있다. According to one embodiment, the porous carbon material may have a lower ratio of ID/IG in a Raman spectrum than that of a wild-type plant-derived porous carbon material of the same species.
일 구체예에 따르면, 상기 다공성 탄소 재료는 BET 표면적이 1450 m2/g 이상일 수 있다. According to one embodiment, the porous carbon material may have a BET surface area of 1450 m 2 /g or more.
일 구체예에 따르면, 상기 다공성 탄소 재료는 야생형 식물로 제조한 다공성 탄소 재료보다 BET 표면적이 10 내지 20%, 11 내지 18%, 12 내지 16%, 또는 약 15.6% 증가한 것일 수 있다.According to one embodiment, the porous carbon material may have a BET surface area increased by 10 to 20%, 11 to 18%, 12 to 16%, or about 15.6% compared to the porous carbon material prepared from wild-type plants.
일 실시예에 따르면, 야생형 포플러 유래 탄소로 제조한 다공성 탄소 재료는 ~1254 m2/g의 BET 표면적을 갖는 반면, 상기 형질전환 포플러 유래 탄소로 제조한 다공성 탄소 재료는 이보다 약 15.6% 늘어난 ~1450 m2/g의 BET 표면적을 갖는 것으로 확인되었다.According to one embodiment, a porous carbon material made from wild-type poplar-derived carbon has a BET surface area of -1254 m 2 /g, whereas a porous carbon material made from transgenic poplar-derived carbon has an increase of about 15.6% to -1450
일 구체예에 따르면, 상기 다공성 탄소 재료는 공극 부피가 0.8 m3/g 이상일 수 있다. According to one embodiment, the porous carbon material may have a pore volume of 0.8 m 3 /g or more.
일 구체예에 따르면, 상기 다공성 탄소 재료는 야생형 식물로 제조한 다공성 탄소 재료보다 공극 부피가 10 내지 20%, 11 내지 18%, 12 내지 16%, 또는 약 15.9% 증가한 것일 수 있다.According to one embodiment, the porous carbon material may have a pore volume increased by 10 to 20%, 11 to 18%, 12 to 16%, or about 15.9% compared to the porous carbon material prepared from wild-type plants.
일 실시예에 따르면, 야생형 포플러 유래 탄소로 제조한 다공성 탄소 재료는 약 0.69 m3/g의 공극 부피를 갖는 반면, 상기 형질전환 포플러 유래 탄소로 제조한 다공성 탄소 재료는 이보다 약 15.9% 늘어난 0.8 m3/g의 공극 부피를 갖는 것으로 확인되었다.According to one embodiment, the porous carbon material made of wild-type poplar-derived carbon has a pore volume of about 0.69 m 3 /g, while the porous carbon material made of transgenic poplar-derived carbon has a pore volume of 0.8 m, which is about 15.9% higher than this. It was found to have a pore volume of 3 /g.
다른 양상은, 상기 다공성 탄소재료를 포함하는 이중층 커패시터 전극을 제공한다. Another aspect provides a double layer capacitor electrode comprising the porous carbon material.
상기 이중층 커패시터 전극은 도전재를 포함할 수 있다. 상기 도전재는 당업계에 공지된 물질이라면 특별히 한정되지 않으며, 예를 들면 흑연, Super C(TIMCAL사), 기상탄화탄소섬유(Vapor Grown Carbon fiber), 카본 나노 튜브, 케첸 블랙(Ketjen black), 덴카 블랙(Denka black), 메조기공카본(mesoporous carbon) 등을 사용할 수 있다. The double layer capacitor electrode may include a conductive material. The conductive material is not particularly limited as long as it is a material known in the art, and for example, graphite, Super C (TIMCAL), vapor grown carbon fiber, carbon nanotube, Ketjen black, Denka Black (Denka black), mesoporous carbon (mesoporous carbon), etc. can be used.
상기 이중층 커패시터 전극은 바인더를 포함할 수 있다. 상기 바인더는 당업계에 공지된 물질이라면 특별히 한정되지 않으며, PTFE(Polytetrafluoroethylene), CMC(Carboxymethylcellulose), PVA (Polyvinylalcohol), PVDF(Polyvinylidenefluoride), PVP(Polyvinylpyrrolidone), MC(메틸 셀룰로오스), SBR(Styrene Butadiene Rubber), 에틸렌-염화비닐 공중합수지, 염화비닐리덴 라텍스, 염소화 수지, 초산 비닐 수지, 폴리비닐 부티랄, 폴리비닐 포름알비스페놀계 에폭시수지, 부타디엔 고무, 이소프렌 고무, 니트릴 부타디엔 고무, 우레탄 고무, 실리콘 고무, 아크릴 고무 등을 사용할 수 있다. The double layer capacitor electrode may include a binder. The binder is not particularly limited as long as it is a material known in the art, PTFE (Polytetrafluoroethylene), CMC (Carboxymethylcellulose), PVA (Polyvinylalcohol), PVDF (Polyvinylidenefluoride), PVP (Polyvinylpyrrolidone), MC (methyl cellulose), SBR (Styrene Butadiene rubber), ethylene-vinyl chloride copolymer resin, vinylidene chloride latex, chlorinated resin, vinyl acetate resin, polyvinyl butyral, polyvinyl formalbisphenol type epoxy resin, butadiene rubber, isoprene rubber, nitrile butadiene rubber, urethane rubber, silicone Rubber, acrylic rubber, etc. can be used.
일 구체예에 따르면, 상기 이중층 커패시터 전극은 0.2 A/g의 전기밀도에서 정전용량이 229 F/g 이상일 수 있다.According to one embodiment, the capacitance of the double-layer capacitor electrode may be 229 F/g or more at an electric density of 0.2 A/g.
일 구체예에 따르면, 상기 이중층 커패시터 전극은 야생형 식물로부터 제조한 다공성 탄소 재료를 포함하는 전극보다 정전용량이 40 내지 100%, 50 내지 90%, 60 내지 80%, 또는 65 내지 75% 증가한 것일 수 있다. According to one embodiment, the double-layer capacitor electrode may have capacitance increased by 40 to 100%, 50 to 90%, 60 to 80%, or 65 to 75% compared to an electrode containing a porous carbon material prepared from a wild type plant. there is.
일 실시예에 따르면, 상기 형질전환 식물에서 유래한 다공성 탄소 재료로 제조한 전극은 야생형 식물에서 유래한 다공성 탄소 재료로 제조한 다공성 탄소 재료로 제조한 전극보다 정전용량이 76.14% 증가한 것으로 확인되었다. According to one embodiment, it was confirmed that the electrode made of the porous carbon material derived from the transgenic plant had a 76.14% increase in capacitance compared to the electrode made of the porous carbon material derived from the wild type plant.
일 구체예에 따른 형질전환 식물 유래 다공성 탄소 재료는 야생형 식물 유래 다공성 탄소 재료보다 비표면적 및 산소 원자 밀도가 크게 증가함으로써 슈퍼커패시터에 사용하기 적합한 전기화학적 특성을 가질 수 있다. The transgenic plant-derived porous carbon material according to one embodiment may have electrochemical properties suitable for use in a supercapacitor because the specific surface area and oxygen atom density are greatly increased compared to those of the wild-type plant-derived porous carbon material.
일 구체예에 따른 형질전환 식물 유래 다공성 탄소 재료로 제조한 전극은 우수한 전기 밀도를 가질 수 있으므로 슈퍼커패시티용 전극으로 사용하기에 적합하다.An electrode made of a transgenic plant-derived porous carbon material according to one embodiment may have excellent electric density, and thus is suitable for use as an electrode for supercapacity.
도 1은 형질전환 포플러 나무로부터 다공성 탄소 재료를 제조하는 과정을 나타낸 것이다.
도 2에서, 도 2A는 일 실시예에 따른 형질전환 포플러와 야생형 포플러의 길이 및 직경을 측정한 결과이고, 도 2B는 셀룰로오스, 헤미셀룰로오스, 및 리그닌의 함량을 나타낸 것이다.
도 3은 형질전환 포플러 또는 야생형 포플러로부터 유래한 다공성 탄소 재료의 미세 구조 및 형태를 SEM으로 확인한 결과이다.
도 4는 형질전환 포플러 또는 야생형 포플러로부터 유래한 다공성 탄소 재료의 라만 스펙트럼 분석 결과를 나타낸 것이다.
도 5는 형질전환 포플러 또는 야생형 포플러로부터 유래한 다공성 탄소 재료의 표면 조성 특성을 X선 광전자 분광법(X-ray photoelectron spectroscopy, XPS)으로 분석한 결과이다.
도 6은 상기 C1s XPS 스펙트럼을 C=C (284.3 eV), C-C (285.1 eV), C-O (286.0 eV) 및 C=O (288.0 eV) 결합의 탄소 원자에 해당하는 4개의 피크로 분해한 결과이다.
도 7은 일 실시예에 따른 다공성 탄소 재료의 N2 흡착/탈착 등온선 및 기공 크기 분포를 나타낸 것이다.
도 8은 일 실시예에 따른 다공성 탄소 재료로 제작한 전극의 CV(Cyclic voltammetry), GCD(Galvanostatic charge-discharge), 정전용량 및 유지를 확인한 결과이다.1 shows a process for preparing a porous carbon material from a transgenic poplar tree.
In Figure 2, Figure 2A is the result of measuring the length and diameter of the transgenic poplar and wild-type poplar according to an embodiment, Figure 2B shows the content of cellulose, hemicellulose, and lignin.
3 is a result of confirming the microstructure and shape of the porous carbon material derived from transgenic poplar or wild-type poplar by SEM.
4 shows the results of Raman spectrum analysis of porous carbon materials derived from transgenic poplar or wild-type poplar.
5 is a result of analyzing the surface composition characteristics of the porous carbon material derived from transgenic poplar or wild-type poplar by X-ray photoelectron spectroscopy (XPS).
6 is a result of decomposing the C1s XPS spectrum into four peaks corresponding to carbon atoms of C=C (284.3 eV), CC (285.1 eV), CO (286.0 eV) and C=O (288.0 eV) bonds. .
7 shows
8 is a result of checking CV (Cyclic voltammetry), GCD (Galvanostatic charge-discharge), capacitance, and retention of an electrode made of a porous carbon material according to an embodiment.
이하 하나 이상의 구체예를 실시예를 통해 보다 상세하게 설명한다. 그러나, 이들 실시예는 하나 이상의 구체예를 예시적으로 설명하기 위한 것으로 본 발명의 범위가 이들 실시예에 한정되는 것은 아니다. Hereinafter, one or more specific examples will be described in more detail through examples. However, these examples are intended to illustrate one or more specific examples, and the scope of the present invention is not limited to these examples.
실험방법Experiment method
1. 형질전환 포플러 제조1. Production of transgenic poplar
Pinus densiflora와 Populus trichocarpa의 cDNA에서 PtrMYB221 및 PdGA20ox1을 인코딩하는 cDNA를 증폭했다. PtrMYB221 및 PdGA20ox1 유전자를 2A 펩타이드(서열번호 4: QLLNFDLLKLAGDVESNPGP)로 연결하여 PdGA20ox1-2A-PtrMYB221 융합 유전자 구조체(construct)를 제작했다. DX15-pMDC32 벡터의 DX15 프로모터의 다운스트림에 상기 융합 유전자 구조체를 삽입했다. cDNAs encoding PtrMYB221 and PdGA20ox1 were amplified from the cDNAs of Pinus densiflora and Populus trichocarpa . PtrMYB221 and PdGA20ox1 genes were ligated with 2A peptide (SEQ ID NO: 4: QLLNFDLLKLAGDVESNPGP) to construct a PdGA20ox1-2A-PtrMYB221 fusion gene construct. The fusion gene construct was inserted downstream of the DX15 promoter in the DX15-pMDC32 vector.
잎 디스크 형질전환-재생 방법(leaf disk transformation-regeneration method)에 의해 잡종 포플러를 형질전환시키기 위해 Agrobacterium tumefaciens 균주 C58에 벡터 구조체(construct)를 도입하였다.A vector construct was introduced into Agrobacterium tumefaciens strain C58 to transform hybrid poplar by the leaf disk transformation-regeneration method.
2. 형질전환 포플러의 생육 2. Growth of transgenic poplar
야생형(Populus alba × Populus glandulosa, cv. BH) 및 형질전환 잡종(hybrid) 포플러는 대한민국 특허공보 제10-2016-0023589호에 기재된 대로 재배되었다. 야생형 및 형질전환 잡종 포플러는 24℃ 또는 LMO(Living Modified Organism) 사이트(위도 37.2N, 경도 126.9E)에서 성장실(16시간 광도, 광도, 150μmol/m/s)의 통제된 조건 하에서 화분에서 재배되었다. LMO 사이트의 나무 샘플은 성장 3개월 후에 수집되었다.Wild type ( Populus alba × Populus glandulosa , cv. BH) and transgenic hybrid poplar were cultivated as described in Korean Patent Publication No. 10-2016-0023589. Wild-type and transgenic hybrid poplars were grown in pots under controlled conditions in a growth chamber (16-h light intensity, light intensity, 150 μmol/m/s) at 24°C or at a Living Modified Organism (LMO) site (latitude 37.2N, longitude 126.9E). It became. Tree samples from the LMO site were collected after 3 months of growth.
3. 셀룰로오스, 헤미셀룰로오스 및 리그닌 간의 비율 결정3. Determination of the ratio between cellulose, hemicellulose and lignin
포플러 샘플에서 세 가지 성분의 양을 결정하였다. 구체적으로, 포플러 시료에서 추출성물질(extractive), 헤미셀룰로오스 및 리그닌을 연속적으로 제거하기 위해 아세톤, 수산화나트륨(sodium hydroxide) 및 황산(sulfuric acid)이 사용되었다. 추출성물질, 헤미셀룰로오스, 리그닌, 셀룰로오스만을 고려하고 각 처리 전후의 질량 변화를 모니터링하여 세 성분 간의 비율을 계산했다.The amounts of the three components were determined in poplar samples. Specifically, acetone, sodium hydroxide and sulfuric acid were used to continuously remove extractives, hemicellulose and lignin from poplar samples. Considering only the extractables, hemicellulose, lignin, and cellulose, and monitoring the mass change before and after each treatment, the ratio between the three components was calculated.
4. 다공성 탄소 재료(porous carbon material) 준비4. Preparation of porous carbon material
형질전환 포플러 및 야생 포플러의 주요 줄기를 절단하여 65℃의 오븐에서 건조시켰다. 건조된 샘플을 분쇄한 다음 40 mesh sieves(425μm)를 통과시켰다. 포플러 시료와 KOH를 1:2의 중량비로 혼합하고 80mL의 증류수를 첨가하였다. 그 다음 혼합물을 120℃의 오븐에서 완전히 건조시켰다. 건조된 샘플을 120℃에서 1시간 동안 안정화시킨 후 N2 flow(200mL/min) 하에서 1시간 동안 800℃(가열 속도 5℃/min)에서 탄화시켰다. N2 흐름하에 상온으로 냉각시킨 후, 샘플 pH가 7에 도달할 때까지 활성탄에 HCl을 첨가하였다. 마지막으로, 샘플을 증류수로 철저히 세척하였다.The main stems of transgenic and wild poplars were cut and dried in an oven at 65°C. The dried sample was ground and then passed through 40 mesh sieves (425 μm). A poplar sample and KOH were mixed in a weight ratio of 1:2, and 80 mL of distilled water was added. The mixture was then dried completely in an oven at 120°C. After stabilizing the dried sample at 120 °C for 1 hour, it was carbonized at 800 °C (
5. 다공성 탄소 재료의 특성 분석 5. Characterization of porous carbon materials
제작된 탄소 재료의 형태는 주사 전자 현미경(SEM; JSM-7600F, JEOL)으로 ~8mm의 작동 거리와 15kV의 가속 전압 조건에서 관찰하였다. 라만 스펙트럼은 360 nm 레이저가 있는 QE-PRO 분광계(Ocean Optics Inc.)를 사용하여 기록되었다. XPS 분석은 Al K-alpha 소스와 함께 Thermo K-Alpha를 사용하여 수행되었다. Survey 스캔은 200 eV의 pass energy를 5회 반복했다. 500 eV의 pass energy는 0.1 eV 분해능으로 사용되었으며 C1s 스캔에 대해 15회 반복되었다. 질소 흡착 등온선(Nitrogen sorption isotherm)은 Micromeritics ASAP 2020 흡착계를 사용하여 -196℃에서 수집되었다. BET(Brunauer-Emmett-Teller) 방정식을 사용하여 표면적을 계산하고 NLDFT(Non-Local Density Functional Theory)를 사용하여 기공 크기 분포를 구했다.The morphology of the fabricated carbon material was observed with a scanning electron microscope (SEM; JSM-7600F, JEOL) at a working distance of ~8 mm and an accelerating voltage of 15 kV. Raman spectra were recorded using a QE-PRO spectrometer (Ocean Optics Inc.) with a 360 nm laser. XPS analysis was performed using Thermo K-Alpha with an Al K-alpha source. The survey scan was repeated 5 times with a pass energy of 200 eV. A pass energy of 500 eV was used with 0.1 eV resolution and repeated 15 times for C1s scans. Nitrogen sorption isotherms were collected at -196 °C using a Micromeritics ASAP 2020 adsorption system. The surface area was calculated using the Brunauer-Emmett-Teller (BET) equation and the pore size distribution was obtained using Non-Local Density Functional Theory (NLDFT).
6. 다공성 탄소 재료를 이용한 탄소 전극 및 코인셀 준비6. Preparation of carbon electrode and coin cell using porous carbon material
H2O에 80 wt% 포플러 유래 활성탄(activated carbon), 10 wt% Ketjen black (KB600JD) 및 10 wt% polytetrafluoroethylene(Sigma Aldrich)을 혼합하였다. 혼합물을 120℃의 진공 오븐에서 밤새 건조시킨 다음 직경 10mm의 디스크로 절단하여 다공성 탄소 전극을 제작하였다. 대조군 시료는 시판되는 활성탄(YP-50F, Kuraray Co. Ltd.)을 사용하여 동일한 방법으로 준비하였다. H 2 O was mixed with 80 wt% poplar-derived activated carbon, 10 wt% Ketjen black (KB600JD) and 10 wt% polytetrafluoroethylene (Sigma Aldrich). The mixture was dried in a vacuum oven at 120 °C overnight and then cut into disks with a diameter of 10 mm to fabricate porous carbon electrodes. Control samples were prepared in the same way using commercially available activated carbon (YP-50F, Kuraray Co. Ltd.).
전해질(4M H2SO4) 및 여과지(~5㎛ 두께, Advantec)로 분리된 2개의 대칭 다공성 탄소 전극(symmetrical porous carbon electrode)으로 2032형 스테인리스강 코인셀을 조립했다. A 2032-type stainless steel coin cell was assembled with two symmetrical porous carbon electrodes separated by electrolyte (4M H 2 SO 4 ) and filter paper (~5 μm thick, Advantec).
7. 전기화학적 특성 분석7. Electrochemical characterization
0.0 내지 0.6 V의 전압 범위에서 10 mV/s에서 potentiostat(SP2, Wonatech)를 사용하여 순환전압전류법(Cyclo-Voltammetry, CV)을 수행했다. Cyclo-Voltammetry (CV) was performed using a potentiostat (SP2, Wonatech) at 10 mV/s in the voltage range of 0.0 to 0.6 V.
정전류 충방전(Galvanostatic charge-discharge, GCD) 테스트는 0.2 내지 20A/g의 전류 밀도 및 0.0 내지 0.6V의 전압 범위에서 배터리 테스트 시스템(WBCS3000Le, Wonatech)을 사용하여 수행되었다. 중량 커패시턴스(gravimetric capacitance) C(F/g)는 C = (2I)/((dV/dt)m)로 계산되었다. 여기서 I은 전류(A), dV/dt는 방전 곡선의 기울기(V/s)이고, m은 전극 질량(g)이다.Galvanostatic charge-discharge (GCD) tests were performed using a battery test system (WBCS3000Le, Wonatech) at current densities of 0.2 to 20 A/g and voltage ranges of 0.0 to 0.6 V. The gravimetric capacitance C(F/g) was calculated as C = (2I)/((dV/dt)m). Here, I is the current (A), dV/dt is the slope of the discharge curve (V/s), and m is the electrode mass (g).
실시예 1: 형질전환 포플러 제조Example 1: Production of transgenic poplar
도 1은 슈퍼커패시터 전극용 형질전환 포플러 유래 다공성 탄소 재료를 제조하는 과정을 나타낸 것이다. 포플러(poplar) 나무는 세계적으로 널리 생육하며 성장률이 높고 유전자가 규명되었으므로 유전자 변형 및 분석이 용이하여 선택되었다. 1 shows a process for preparing a porous carbon material derived from transgenic poplar for supercapacitor electrodes. Poplar trees were selected because they grow widely worldwide, have high growth rates, and are easy to genetically modify and analyze because their genes have been identified.
상기 실험방법으로 생체 활성 지베렐린 합성 경로의 속도 제한 단계를 촉매하여 줄기 신장을 유발하는 PdGA20ox1과 리그닌 생합성을 부정적으로 조절하는 전사 인자 PtrMYB221을 목부조직 특이적으로 발현시킨 형질전환 포플러를 얻었다. 형질전환 포플러를 분쇄(grind)하여 알칼리 활성화(alkali activate)하고 탄화(carbonized)시켰다.Through the above experimental method, transgenic poplars expressing PdGA20ox1, which induces stem elongation by catalyzing the rate-limiting step of the bioactive gibberellin synthesis pathway, and PtrMYB221, a transcription factor that negatively regulates lignin biosynthesis, were expressed specifically in xylem tissue. The transformed poplar was ground, alkali activated, and carbonized.
형질전환 포플러는 목질계 바이오매스의 양이 증가하였다. 도 2A에 따르면, 형질전환 포플러 샘플(n = 6)과 야생형 포플러 샘플(n = 9)을 비교하면 형질전환 포플러의 높이와 직경이 각각 49.7% 및 24.6% 증가했다. Transgenic poplars increased the amount of lignocellulosic biomass. According to Fig. 2A, comparing the transgenic poplar sample (n = 6) and the wild-type poplar sample (n = 9), the height and diameter of the transgenic poplar increased by 49.7% and 24.6%, respectively.
포플러 샘플(n = 3)의 조성도 크게 변화하였다. 도 2B에 따르면, 형질전환 포플러의 리그닌 함량은 약 37.7% 감소한 반면, 셀룰로오스 분획은 야생형 포플러에 비해 약 22.5% 증가했다.The composition of the poplar samples (n = 3) also varied greatly. According to Fig. 2B, the lignin content of transgenic poplar decreased by about 37.7%, while the cellulose fraction increased by about 22.5% compared to wild-type poplar.
바이오매스의 셀룰로오스 분획의 증가와 리그닌 분획의 감소가 이를 탄화시켜 제조한 다공성 탄소의 전기화학적 성질에 미치는 영향은 알려진 바가 없다.The effect of increasing the cellulose fraction of biomass and decreasing the lignin fraction on the electrochemical properties of porous carbon prepared by carbonizing it is unknown.
실시예 2: 다공성 탄소 샘플의 특성Example 2: Characteristics of Porous Carbon Samples
다공성 탄소 샘플의 표면 미세 구조 및 형태는 SEM으로 확인하였다. The surface microstructure and morphology of the porous carbon samples were confirmed by SEM.
도 3에 따르면, 형질전환 포플러 유래 또는 야생형 포플러 유래 다공성 탄소는 모두 3차원적으로 상호 연결된 기공 구조를 가지지만, 형질전환 포플러 유래 탄소는 작은 공동(cavity)의 밀도가 더 높았고, 이로 인해 표면적이 더 넓어져 전하 저장을 향상시킬 것으로 예상되었다.According to FIG. 3, the porous carbon derived from transgenic poplar or wild-type poplar both had a three-dimensionally interconnected pore structure, but the carbon derived from transgenic poplar had a higher density of small cavities, which resulted in a higher surface area. It was expected that being wider would improve charge storage.
야생 및 형질전환 포플러에서 파생된 다공성 탄소의 라만 스펙트럼을 분석하였다. 도 4에 따르면, 두 탄소 모두 ~1583 cm-1의 G 밴드와 ~1315 cm-1의 D 밴드에 해당하는 두 개의 명확한 피크를 나타냈다. Raman spectra of porous carbon derived from wild and transgenic poplars were analyzed. According to FIG. 4, both carbons showed two distinct peaks corresponding to the G band of ~1583 cm -1 and the D band of ~1315 cm -1 .
D 및 G 밴드의 강도 비율로 다공성 탄소의 무질서 수준을 특성화하였다. 형질전환 포플러 유래 다공성 탄소의 ID/IG 비율은 야생형 포플러 유래 다공성 탄소의 ID/IG 비율보다 낮았다. 이는 β-1,4 glycosidic bond 및 사슬간 수소 결합(interchain hydrogen bond)을 갖는 정렬된 셀룰로오스(ordered cellulose)의 분율(fraction)이 더 높기 때문일 수 있다. 흑연화 정도(graphitization degree)가 높을수록 전자 전도성이 향상되는 것으로 알려져 있다.The level of disorder in porous carbon was characterized by the intensity ratio of the D and G bands. The ID/IG ratio of porous carbon derived from transgenic poplar was lower than that of porous carbon derived from wild-type poplar. This may be due to the higher fraction of ordered cellulose with β-1,4 glycosidic bonds and interchain hydrogen bonds. It is known that the higher the graphitization degree, the higher the electronic conductivity.
X선 광전자 분광법(X-ray photoelectron spectroscopy, XPS)으로 야생 및 형질전환 포플러에서 유래한 다공성 탄소 재료의 표면 조성의 특성을 분석하였다. 도 5에 따르면, 다공성 탄소는 미량 불순물(trace impurities) 없이 주로 C와 O로 구성되어 있었다. 형질전환 포플러 유래 다공성 탄소 재료의 산소 대 탄소 비율(O/C)은 야생형 포플러 유래 다공성 탄소 재료보다 18.9% 높았다. 이 차이는 형질전환 포플러의 셀룰로오스 비율이 더 높기 때문일 수 있다. 셀룰로오스는 리그닌보다 산소 원자를 더 높은 밀도로 포함하며, 산소 원자는 리그닌에서 셀룰로오스로 이동할 수 있기 때문이다.The surface composition of porous carbon materials derived from wild and transgenic poplars was characterized by X-ray photoelectron spectroscopy (XPS). According to FIG. 5, porous carbon was mainly composed of C and O without trace impurities. The oxygen-to-carbon ratio (O/C) of the transgenic poplar-derived porous carbon material was 18.9% higher than that of the wild-type poplar-derived porous carbon material. This difference may be due to the higher percentage of cellulose in transgenic poplar. This is because cellulose contains a higher density of oxygen atoms than lignin, and oxygen atoms can migrate from lignin to cellulose.
C1s XPS 스펙트럼을 C=C (284.3 eV), C-C (285.1 eV), C-O (286.0 eV) 및 C=O (288.0 eV) 결합의 탄소 원자에 해당하는 4개의 피크로 분해하였다. 도 6에 따르면, 두 샘플 모두 동일한 유형의 화학 결합을 포함했지만 상대적 비율은 상당한 차이가 있었다. 특히, 형질전환 포플러 유래 탄소 재료는 C-C 및 C-O 결합에 대한 신호의 강도가 야생형 포플러 유래 탄소 재료보다 더 높았다. The C1s XPS spectrum was resolved into four peaks corresponding to the carbon atoms of C=C (284.3 eV), C-C (285.1 eV), C-O (286.0 eV) and C=O (288.0 eV) bonds. According to Fig. 6, both samples contained the same type of chemical bonds, but the relative proportions were significantly different. In particular, the carbon material derived from transgenic poplar showed higher signal intensity for C-C and C-O bonds than the carbon material derived from wild-type poplar.
도 7A에 따르면, 다공성 탄소의 N2 흡착/탈착 등온선은 낮은 상대 압력에서 현저한 흡착이 일어나 유형 I 거동(Type I behavior)을 나타냈다. 상대압력이 높아짐에 따라 미세 기공(micropores)과 작은 메조 기공(small mesopores)에 의해 고원이 형성되었다.According to FIG. 7A, the N 2 adsorption/desorption isotherm of porous carbon showed Type I behavior with significant adsorption occurring at a low relative pressure. As the relative pressure increased, a plateau was formed by micropores and small mesopores.
도 7B에 따르면, 기공 크기 분포는 두 다공성 탄소가 모두 작은 메조 기공(mesopore)(2-4 nm)과 미세 기공(micropore)(<2 nm)을 가지고 있음을 나타낸다. 그러나 형질전환 포플러 유래 다공성 탄소는 야생 포플러 유래 탄소(~1254 m2/g 및 0.69 cm3/g)보다 더 큰 공극 부피(0.8 cm3/g)와 비표면적(~1450 m2/g)을 가졌다. 이는 글루코스의 산소가 CO2, CO 및 H2로 방출됨으로써 셀룰로오스의 더 많은 부분에서 기공을 형성될 수 있기 때문으로 생각된다. 또한 형질전환 포플러 유래 다공성 탄소는 이온이 접근할 수 있는 영역이 더 넓어졌으므로 에너지 저장 기능이 향상될 것으로 예상된다.According to Fig. 7B, the pore size distribution indicates that both porous carbons have small mesopores (2-4 nm) and micropores (<2 nm). However, the porous carbon from transgenic poplar has a larger pore volume (0.8 cm 3 /g) and specific surface area (~1450 m 2 /g) than wild poplar-derived carbon (~1254 m 2 /g and 0.69 cm 3 /g). had This is thought to be because the oxygen of glucose is released as CO 2 , CO and H 2 so that pores can be formed in more parts of the cellulose. In addition, the porous carbon derived from transgenic poplar is expected to have an improved energy storage function because the area accessible to ions is wider.
실시예 3: 다공성 탄소의 전기화학적 특성Example 3: Electrochemical properties of porous carbon
CV(Cyclic voltammetry) 및 GCD(Galvanostatic charge-discharge)를 분석하여 포플러 유래 다공성 탄소로 제조한 전극의 전기화학적 성능을 조사하였다. 이하 형질전환 포플러 유래 전극 및 야생형 포플러 유래 전극으로 약칭할 수 있다. The electrochemical performance of electrodes made of poplar-derived porous carbon was investigated by analyzing cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD). Hereinafter, it can be abbreviated as an electrode derived from transgenic poplar and an electrode derived from wild-type poplar.
도 8A에 따르면, 각 샘플의 CV 곡선은 준 직사각형 모양을 나타냈으며, 빠른 이온 확산과 이상적인 전기 이중층 용량 거동(electrical double-layer capacitive behavior)을 나타냈다. 0.6V 근처의 작은 기울기는 산소 작용기의 산화환원에서 기인한 것일 수 있다. 실험결과에 따르면, 형질전환 포플러 유래 전극은 야생형 유래 포플러 유래 전극보다 훨씬 더 큰 CV 면적을 가지며, 정전용량이 더 큰 것으로 확인되었다.8A, the CV curves of each sample exhibited a quasi-rectangular shape, exhibiting fast ion diffusion and ideal electrical double-layer capacitive behavior. The small slope around 0.6 V may be due to redox of oxygen functional groups. According to the experimental results, it was confirmed that the transgenic poplar-derived electrode had a much larger CV area and higher capacitance than the wild-type poplar-derived electrode.
이러한 거동은 GCD 측정으로도 확인되었다. 도 8B에 따르면, 형질전환 포플러 유래 전극의 GCD 곡선은 서로 다른 전류 밀도에서 전형적인 대칭 삼각형 모양을 가지며, 이는 2차 산화환원 반응이 없거나 내부 저항이 높다는 것을 의미한다. This behavior was also confirmed by GCD measurements. According to Fig. 8B, the GCD curves of the transgenic poplar-derived electrodes have a typical symmetric triangular shape at different current densities, which means that there is no secondary redox reaction or high internal resistance.
형질전환 포플러, 야생 포플러 및 상업용 활성탄(commercial activated carbon; YP-50F, Kuraray Co. Ltd.)에서 유래한 전극의 비정전용량을 전류 밀도와 비교했다. 도 8C에 따르면, 0.2 A/g에서 형질전환 포플러 유래 전극의 정전용량은 229.46 F/g으로 야생 포플러 및 상업용 다공성 탄소 유래 전극보다 각각 76.14% 및 60.96% 더 높았다. 특히, 형질전환 포플러 유래 전극은 조사된 모든 속도(0.2-20 A/g)에서 다른 두 샘플보다 상당히 높은 정전용량을 보여주었다. 이러한 향상된 성능은 높은 셀룰로오스 분율에서 유래하는 더 큰 표면적과 더 높은 밀도의 산소 작용기에 의한 것일 수 있다. 더 큰 표면적은 하전된 이온을 수용할 더 많은 공간을 제공하며, 산소 작용기는 전해질에 의한 탄소 표면의 습윤성을 향상시킬 수 있다. 야생 포플러 유래 전극의 커패시턴스는 비교적 높은 전류 밀도(5-20A/g)에서 상용 다공성 탄소의 커패시턴스보다 우수한 것으로 확인되었다. 이 연구에 사용된 상업용 다공성 탄소(commercial porous carbon)는 야생 포플러에서 추출한 다공성 탄소보다 평균 기공 크기가 작고 중간 기공의 수가 적었다. 따라서 기공의 이온 접근이 제한됨으로 인해 전류 밀도가 증가함에 따라 정전 용량 강하가 빠르다. The specific capacitance of electrodes derived from transgenic poplar, wild poplar and commercial activated carbon (YP-50F, Kuraray Co. Ltd.) was compared with the current density. According to Fig. 8C, the capacitance of the transgenic poplar-derived electrode at 0.2 A/g was 229.46 F/g, 76.14% and 60.96% higher than the wild poplar and commercial porous carbon-derived electrodes, respectively. In particular, the transgenic poplar-derived electrode showed significantly higher capacitance than the other two samples at all rates investigated (0.2–20 A/g). This improved performance may be due to the higher surface area and higher density of oxygen functional groups resulting from the higher cellulose fraction. A larger surface area provides more space to accommodate charged ions, and oxygen functional groups can enhance the wettability of the carbon surface by electrolytes. The capacitance of wild poplar-derived electrodes was found to be superior to that of commercially available porous carbons at relatively high current densities (5–20 A/g). The commercial porous carbon used in this study had a smaller average pore size and fewer mesopores than the porous carbon extracted from wild poplar. Therefore, the capacitance drop is rapid as the current density increases due to the limited ion access in the pore.
도 8D에 따르면, 야생 포플러 유래 전극 및 형질전환 포플러 유래 전극 모두 1A/g에서 10,000회 이상의 우수한 정전용량 유지를 나타냈다.According to Fig. 8D, both the wild poplar-derived electrode and the transgenic poplar-derived electrode exhibited excellent capacitance retention of 10,000 cycles or more at 1 A/g.
<110> University-Industry Cooperation Group of Kyung Hee University <120> Transgenic plant-derived porous carbon material and super capacitor using same <130> CDP2021-0875 <160> 4 <170> KoPatentIn 3.0 <210> 1 <211> 1107 <212> DNA <213> Artificial Sequence <220> <223> PdGA20ox1 (Pinus densiflora Gibberellin 20-oxidase 1) <400> 1 atgggtactt cgactgtgag tgggccaaac gtgccagtgt tgttcgatgc tagtattctg 60 caacgagagg agaagatgcc tgaggtattt gtttggcccc aagtggatcg accctccaca 120 gatttggcgt tgaagggaag ggagacagag gtgccattgc cgattatcga tttgggcgga 180 ttctggaaaa atgatgaaaa ggcaaccaaa gaagcgtcag acgttatagg gaaagcctgt 240 gtggaacatg gtttctttca ggtcatcaac catcaagtct ctccagacct cctcactgct 300 gctcatcaac acatcagttt gttttttagt ttgagtttag tggaaaaacg aagggctcaa 360 aggaagcttg gcgagagctg tggatatgcc agtagtttta cggatcgctt tgcaaataaa 420 ctaccatgga aggagacact gtctttcgag cacagtccct cttcagacgt tcgtgactat 480 tttgtcaaag ctatgggtga agattttcaa gacgctggaa atgtattcaa agagtactgt 540 gaagcaatgg aatgcttggc tcttggattg atggagttgt tgggaatgag cctcggaata 600 gggcgtctgc atcttcggaa attttttgaa ggtggcaact caataatgag gttgaactat 660 tatcctcctt gtgcgcagcc aaatctgaca cttgggactg gtccccattg cgatccgaca 720 tcccttactc tccttcatct ggacgaagtg ggaggtctgg agattttcat aaataataag 780 tggcattctg tgcgacccaa cactgatgcc ttcgttgtca acatcggaga cacctttatg 840 gcactgtcca atggtaaata caagagctgc ctccacagag cagtggtgaa caagacaaca 900 cctcgcaaat cactggcatt tttcctgaac ccaccatatg acaaaattgt acgacctcca 960 gatgatcttt tggattctga tcatcctcga aaatatccag atttcacgtg gcctgtgttc 1020 ttggagttca ctcagaaaca ctacagatca gacatgaata ctcttgcagc ttttcagaaa 1080 tggttcacct caagaaacca gccataa 1107 <210> 2 <211> 807 <212> DNA <213> Artificial Sequence <220> <223> PtrMYB221 <400> 2 atgggaaggt ctccttgctg tgaaaaagct catacaaaca aaggcgcatg gactaaggaa 60 gaagatgatc gccttattgc ttacattaga acccacggtg aaggttgctg gcgttcactt 120 cctaaagctg ctggccttct aagatgcggc aagagctgca gacttcgttg gatcaactat 180 ttaagacctg accttaaacg tggcaatttt actgaagaag aagatgagct cattatcaaa 240 ctccatagtc tcctcggcaa caaatggtca cttatagccg gaaggttacc agggagaaca 300 gataatgaga taaagaatta ttggaacaca catataagaa ggaagctctt gaatagaggc 360 atagatcctg cgactcatag gccactcaat gaaccagccc aagaagcttc aacaacaata 420 tctttcagca ctactacctc agttaaagaa gagtcgttga gttctgttaa agaggaaagt 480 aataaggaga agataattag cgcagctgct tttatatgca aagaagagaa aaccccagtt 540 caagaaaggt gtccagactt gaatcttgaa cttagaatta gccttccttg ccaaaaccag 600 cctgatcgtc accaggcatt caaaactgga ggaagtacaa gtctttgttt tgcttgcagc 660 ttggggctac aaaacagcaa ggactgcagt tgcagtgtca ttgtgggtac tattggaagc 720 agcagtagtg ctggctccaa aactggctat gacttcttag ggatgaaaag tggtgtgttg 780 gattatagag gtttggagat gaaatga 807 <210> 3 <211> 1025 <212> DNA <213> Artificial Sequence <220> <223> DX15 promoter <400> 3 ttcccccttt tggttcaatg ccttttattc ttccaaaatt atttcatatt ttgtatccgg 60 aggacatatt tgtttcaaaa ggtgtcagaa aatcaaagcc cattgaaaat atataaacat 120 atatagatat aaaaactcaa gggttcattc caaaatataa gaacaaactg attgaattaa 180 tttgttattt taagaacact gtctatatgt ttatatagtg ggaggtagtg ttttttaaat 240 catatactaa cttattataa aaataaatca taaaaaagga acctcaagca tcccctggta 300 agctcgtatg taggaatact cggagatcaa atgtccgaat gtcaaatgtt aaggcaagtg 360 aaatatccct gactttttag caagcaaatt gttgagtagc taaaatgaat tattttaata 420 tttttaaatc attttaatat attaatatta aaaaaaatta aatatttttt ttaatacatt 480 ttcaataaca aacactttaa aatataatct ttgtcacact cttaaacagt aacagcagaa 540 agcatatgtg agtgatatag ctatagttgc tgtttgacac ggacaatctc catctaaatt 600 catgaataat aaagttttgc ctacacaccc acttgaaatc tcctcctagt tttcctgatt 660 tgccatgcta actacaagaa caagatgcta gctagtatct tgttctgtct ctcgctctct 720 ctctatctct ccagttgata gttgatagtt gatagttgat agctgatacc ctcccacctt 780 tcccagaaag atgattgagg aactagtcac tgtgttcgtg taactaatac tgttcatggc 840 acctaacttg atcctctctt caccagacca ctataaaaac cctatctgtc ctcctcataa 900 tcatatcact acacccaaca cttctgcaag cacaactcca ttcaagaaca tcaagagtat 960 aggccgccgc tgcaacaaaa cagcactcct agctacttca agatgaggcc acaatctttc 1020 atctt 1025 <210> 4 <211> 20 <212> PRT <213> Artificial Sequence <220> <223> 2A peptide <400> 4 Gln Leu Leu Asn Phe Asp Leu Leu Lys Leu Ala Gly Asp Val Glu Ser 1 5 10 15 Asn Pro Gly Pro 20 <110> University-Industry Cooperation Group of Kyung Hee University <120> Transgenic plant-derived porous carbon material and super capacitor using the same <130> CDP2021-0875 <160> 4 <170> KoPatentIn 3.0 <210> 1 <211> 1107 <212> DNA <213> artificial sequence <220> <223> PdGA20ox1 (Pinus densiflora Gibberellin 20-oxidase 1) <400> 1 atgggtactt cgactgtgag tgggccaaac gtgccagtgt tgttcgatgc tagtattctg 60 caacgagagg agaagatgcc tgaggtattt gtttggcccc aagtggatcg accctccaca 120 gatttggcgt tgaagggaag ggagacagag gtgccattgc cgattatcga tttgggcgga 180 ttctggaaaa atgatgaaaa ggcaaccaaa gaagcgtcag acgttatagg gaaagcctgt 240 gtggaacatg gtttctttca ggtcatcaac catcaagtct ctccagacct cctcactgct 300 gctcatcaac acatcagttt gttttttagt ttgagtttag tggaaaaacg aagggctcaa 360 aggaagcttg gcgagagctg tggatatgcc agtagtttta cggatcgctt tgcaaataaa 420 ctaccatgga aggagacact gtctttcgag cacagtccct cttcagacgt tcgtgactat 480 tttgtcaaag ctatgggtga agattttcaa gacgctggaa atgtattcaa agagtactgt 540 gaagcaatgg aatgcttggc tcttggattg atggagttgt tgggaatgag cctcggaata 600 gggcgtctgc atcttcggaa attttttgaa ggtggcaact caataatgag gttgaactat 660 tatcctcctt gtgcgcagcc aaatctgaca cttgggactg gtccccattg cgatccgaca 720 tcccttactc tccttcatct ggacgaagtg ggaggtctgg agattttcat aaataataag 780 tggcattctg tgcgacccaa cactgatgcc ttcgttgtca acatcggaga cacctttatg 840 gcactgtcca atggtaaata caagagctgc ctccacagag cagtggtgaa caagacaaca 900 cctcgcaaat cactggcatt tttcctgaac ccaccatatg acaaaattgt acgacctcca 960 gatgatcttt tggattctga tcatcctcga aaatatccag atttcacgtg gcctgtgttc 1020 ttggagttca ctcagaaaca ctacagatca gacatgaata ctcttgcagc ttttcagaaa 1080 tggttcacct caagaaacca gccataa 1107 <210> 2 <211> 807 <212> DNA <213> artificial sequence <220> <223> PtrMYB221 <400> 2 atgggaaggt ctccttgctg tgaaaaagct catacaaaca aaggcgcatg gactaaggaa 60 gaagatgatc gccttattgc ttacattaga acccacggtg aaggttgctg gcgttcactt 120 cctaaagctg ctggccttct aagatgcggc aagagctgca gacttcgttg gatcaactat 180 ttaagacctg accttaaacg tggcaatttt actgaagaag aagatgagct cattatcaaa 240 ctccatagtc tcctcggcaa caaatggtca cttatagccg gaaggttacc agggagaaca 300 gataatgaga taaagaatta ttggaacaca catataagaa ggaagctctt gaatagaggc 360 atagatcctg cgactcatag gccactcaat gaaccagccc aagaagcttc aacaacaata 420 tctttcagca ctactacctc agttaaagaa gagtcgttga gttctgttaa agaggaaagt 480 aataaggaga agataattag cgcagctgct tttatatgca aagaagagaa aaccccagtt 540 caagaaaggt gtccagactt gaatcttgaa cttagaatta gccttccttg ccaaaaccag 600 cctgatcgtc accaggcatt caaaactgga ggaagtacaa gtctttgttt tgcttgcagc 660 ttggggctac aaaacagcaa ggactgcagt tgcagtgtca ttgtgggtac tattggaagc 720 agcagtagtg ctggctccaa aactggctat gacttcttag ggatgaaaag tggtgtgttg 780 gattatagag gtttggagat gaaatga 807 <210> 3 <211> 1025 <212> DNA <213> artificial sequence <220> <223> DX15 promoter <400> 3 ttcccccttt tggttcaatg cctttattc ttccaaaatt atttcatatt ttgtatccgg 60 aggacatatt tgtttcaaaa ggtgtcagaa aatcaaagcc cattgaaaat atataaacat 120 atatagatat aaaaactcaa gggttcattc caaaatataa gaacaaactg attgaattaa 180 tttgttattt taagaacact gtctatatgt ttatatagtg ggaggtagtg ttttttaaat 240 catatactaa cttattataa aaataaatca taaaaaagga acctcaagca tcccctggta 300 agctcgtatg taggaatact cggagatcaa atgtccgaat gtcaaatgtt aaggcaagtg 360 aaatatccct gactttttag caagcaaatt gttgagtagc taaaatgaat tattttaata 420 tttttaaatc attttaatat attaatatta aaaaaaatta aatatttttt ttaatacatt 480 ttcaataaca aacactttaa aatataatct ttgtcacact cttaaacagt aacagcagaa 540 agcatatgtg agtgatatag ctatagttgc tgtttgacac ggacaatctc catctaaatt 600 catgaataat aaagttttgc ctacacaccc acttgaaatc tcctcctagt tttcctgatt 660 tgccatgcta actacaagaa caagatgcta gctagtatct tgttctgtct ctcgctctct 720 ctctatctct ccagttgata gttgatagtt gatagttgat agctgatacc ctcccacctt 780 tcccagaaag atgattgagg aactagtcac tgtgttcgtg taactaatac tgttcatggc 840 acctaacttg atcctctctt caccagacca ctataaaaac cctatctgtc ctcctcataa 900 tcatatcact acacccaaca cttctgcaag cacaactcca ttcaagaaca tcaagagtat 960 aggccgccgc tgcaacaaaa cagcactcct agctacttca agatgaggcc acaatctttc 1020 atctt 1025 <210> 4 <211> 20 <212> PRT <213> artificial sequence <220> <223> 2A peptide <400> 4 Gln Leu Leu Asn Phe Asp Leu Leu Lys Leu Ala Gly Asp Val Glu Ser 1 5 10 15 Asn Pro Gly Pro 20
Claims (9)
상기 형질전환 식물은 PdGA20ox1 (Pinus densiflora Gibberellin 20-oxidase 1) 유전자; 및 PtrMYB221 유전자가 DX15 프로모터에 의해 줄기 특이적으로 과발현된 형질전환 식물인,
다공성 탄소 재료.A porous carbon material prepared by alkali activation and carbonization of lignocellulosic biomass obtained from transgenic plants,
The transgenic plant has a PdGA20ox1 (Pinus densiflora Gibberellin 20-oxidase 1) gene; and a transgenic plant in which the PtrMYB221 gene is stem-specifically overexpressed by the DX15 promoter.
Porous carbon materials.
상기 형질전환 식물은 초본 식물 또는 목본 식물인,
다공성 탄소 재료.According to claim 1,
The transgenic plant is a herbaceous plant or a woody plant,
Porous carbon materials.
다공성 탄소 재료.The method of claim 1, wherein the PdGA20ox1 gene consists of the sequence of SEQ ID NO: 1, and the PtrMYB221 gene consists of the sequence of SEQ ID NO: 2,
Porous carbon materials.
상기 형질전환 식물은 동종의 야생형 식물보다 셀룰로오스 함량이 증가하고 리그닌의 함량이 감소한 것인,
다공성 탄소 재료.According to claim 1,
The transgenic plant has an increased cellulose content and a reduced lignin content than wild-type plants of the same species,
Porous carbon materials.
상기 다공성 탄소 재료는 라만 스펙트럼에서 ID/IG의 비율이 동종의 야생형 식물 유래 다공성 탄소 재료보다 낮은 것인,
다공성 탄소 재료.According to claim 1,
The porous carbon material has a ratio of ID / IG in the Raman spectrum lower than that of the wild-type plant-derived porous carbon material of the same species,
Porous carbon materials.
상기 다공성 탄소 재료는 야생형 식물로 제조한 다공성 탄소 재료보다 BET 표면적이 10 내지 20% 증가한 것인,
다공성 탄소 재료.According to claim 1,
The porous carbon material has a BET surface area increased by 10 to 20% compared to the porous carbon material prepared from wild-type plants,
Porous carbon materials.
상기 다공성 탄소 재료는 야생형 식물로 제조한 다공성 탄소 재료보다 공극 부피가 10 내지 20% 증가한 것인,
다공성 탄소 재료.According to claim 1,
The porous carbon material has a pore volume increased by 10 to 20% compared to the porous carbon material prepared from wild-type plants.
Porous carbon materials.
상기 이중층 커패시터 전극은 야생형 식물에서 유래한 다공성 탄소 재료를 포함하는 전극보다 정전용량이 40 내지 100% 증가한 것인,
이중층 커패시터 전극.
According to claim 8,
The double-layer capacitor electrode has a capacitance increased by 40 to 100% compared to an electrode containing a porous carbon material derived from a wild-type plant,
double-layer capacitor electrodes.
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