KR20180096953A - The metal coating layer of the microbial fuel cell was replaced with a carbon nano fiber electrode - Google Patents

The metal coating layer of the microbial fuel cell was replaced with a carbon nano fiber electrode Download PDF

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KR20180096953A
KR20180096953A KR1020170023390A KR20170023390A KR20180096953A KR 20180096953 A KR20180096953 A KR 20180096953A KR 1020170023390 A KR1020170023390 A KR 1020170023390A KR 20170023390 A KR20170023390 A KR 20170023390A KR 20180096953 A KR20180096953 A KR 20180096953A
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fuel cell
microbial fuel
electrode
carbon
metal coating
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장순웅
주현종
김성수
엄한기
최유현
김성철
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경기대학교 산학협력단
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8647—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites
    • H01M4/8657—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites layered
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C18/00—Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating
    • C23C18/16—Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating by reduction or substitution, e.g. electroless plating
    • C23C18/18—Pretreatment of the material to be coated
    • C23C18/20—Pretreatment of the material to be coated of organic surfaces, e.g. resins
    • C23C18/28—Sensitising or activating
    • C23C18/30—Activating or accelerating or sensitising with palladium or other noble metal
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C18/00—Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating
    • C23C18/16—Chemical coating by decomposition of either liquid compounds or solutions of the coating forming compounds, without leaving reaction products of surface material in the coating; Contact plating by reduction or substitution, e.g. electroless plating
    • C23C18/31—Coating with metals
    • C23C18/42—Coating with noble metals
    • C23C18/44—Coating with noble metals using reducing agents
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8817—Treatment of supports before application of the catalytic active composition
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8825—Methods for deposition of the catalytic active composition
    • H01M4/8846—Impregnation
    • H01M4/885—Impregnation followed by reduction of the catalyst salt precursor
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8878—Treatment steps after deposition of the catalytic active composition or after shaping of the electrode being free-standing body
    • H01M4/8882—Heat treatment, e.g. drying, baking
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/92—Metals of platinum group
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/16—Biochemical fuel cells, i.e. cells in which microorganisms function as catalysts
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y40/00—Manufacture or treatment of nanostructures
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y02E60/527—
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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Abstract

The present invention relates to a method for manufacturing an electrode applicable to an oxidizing electrode and a reducing electrode in order to increase the efficiency of production of electricity produced in a microbial fuel cell. Accordingly, carbon-based nanofibers are manufactured and palladium (Pd) is coated on the nanofibers to be applied to the microbial fuel cell. The carbon-based nanofibers according to the present invention facilitate the formation of microbial membranes in the microbial fuel cell and can reduce the voltage drop due to resistance loss by coating a metal catalyst (Pd, Palladium) on the surface. Particularly, the present invention can increase the power production efficiency in the conventional microbial fuel cell since the catalyst metal coating can be performed in the conventional carbon fibers.

Description

미생물 연료전지의 금속코팅 탄소기반 나노섬유 전극 개발{The metal coating layer of the microbial fuel cell was replaced with a carbon nano fiber electrode}BACKGROUND OF THE INVENTION 1. Field of the Invention [0001] The present invention relates to a metal-coated carbon-based nanofiber electrode for a microbial fuel cell,

본 발명은 미생물 연료전지 내 전기생산효율 증가를 위한 전극소재 제조에 관한 것으로써 보다 상세하게는 전기방사를 이용한 탄소기반의 나노섬유를 제조하고 제조된 섬유 표면에 금속촉매 코팅방법에 관한 것이다.The present invention relates to the production of electrode materials for increasing the electrical production efficiency in a microbial fuel cell, and more particularly, to a method of coating a metal catalyst on a fiber surface by preparing carbon-based nanofibers using electrospinning.

미생물연료전지(microbial fuel cell, MFC)는 미생물을 촉매로 이용함으로써 대상물질의 화학에너지를 전기에너지로 전환하는 장치를 의미한다. 폐수 내 유기물 및 무기물을 에너지원으로 사용할 수 있어 대체에너지 기술 중 하나로 주목 받고 있으며 MFC를 이용하여 폐수 내 유기물 및 영양염류의 처리와 전기생산을 동시에 가능하게 하며, 2차오염물질이 생성되지 않는 점에서 매우 혁신적인 기술로 평가되고 있다. A microbial fuel cell (MFC) is a device that converts the chemical energy of a substance into electrical energy by using a microorganism as a catalyst. It is one of the alternative energy technologies because it can use organic and inorganic materials in the wastewater as an energy source. It makes it possible to simultaneously treat organic matter and nutrients in wastewater by using MFC and produce electricity at the same time. Is considered a very innovative technology.

미생물 연료전지는 산화전극부(Anode chamber), 환원전극부(Cathode chamber) 및 이온교환분리막(Separator)로 구성되어 있다. 혐기성 및 무산소조건의 산화전극부에서 미생물에 의해 유기물이 분해되고, 수소 및 전자가 발생한다. 전자의 경우 외부도선을 따라 산화전극부에서 환원전극부로 이동하게 되고, 수소이온의 경우 이온분리막을 통과하여 환원전극부로 이동하게 된다. 환원전극부로 이동한 전자와 수소이온은 환원 전극부에서 공급되는 산소이온, 오존, 질산염과 같은 전자수용체와 반응하여 물이 생성된다. The microbial fuel cell is composed of an anode chamber, a cathodic chamber, and an ion exchange separator. Organic matter is decomposed by microorganisms in the oxidizing electrode part under anaerobic and anoxic conditions, and hydrogen and electrons are generated. In the case of electrons, the electrons move from the oxidized electrode portion to the reduced electrode portion along the outer conductor, and the hydrogen ions move to the reducing electrode portion through the ion-exchanged membrane. The electrons and hydrogen ions migrating to the reduction electrode portion react with electron acceptors such as oxygen ions, ozone, and nitrate supplied from the reduction electrode portion, and water is generated.

미생물 전극 재료의 필요조건으로는 높은 전기전도성, 비부식성, 높은표면적, 다공성 및 낮은 세공의 막힘성 등이 있으며, 이러한 특성 중 연료전지 전극의 가정 중요한 특성은 높은 전기전도성이다. 일반적으로 탄소종이, 탄소천, 및 발포형 등의 탄소물질은 높은 전기전도성을 띠고 있으며, 미생물 성장에 매우 적절한 조건을 제공하는 것으로 알려져 있다.   The requirements for the microbial electrode material include high electrical conductivity, noncorrosive, high surface area, porosity, and clogging of low pores. Among these properties, a high characteristic of the fuel cell electrode is the high electrical conductivity. Generally, carbon materials such as carbon paper, carbon cloth, and foaming have high electrical conductivity and are known to provide very suitable conditions for microbial growth.

전극재료로 사용되는 탄소물질에 다양한 종류의 금속 및 촉매를 코팅함으로써 기존 상용화된 전극보다 높은 전력을 생산함으로써 전기생산효율을 증가시킬 수 있으나 코팅 금속의 경제성으로 인해 상용화가 어려운 실정이다.  By coating various kinds of metal and catalyst on the carbon material used as the electrode material, it is possible to increase the electric production efficiency by producing higher electric power than the conventional commercialized electrode, but commercialization due to the economical efficiency of the coating metal is difficult.

따라서 미생물연료전지를 실용화 하기 위해서는 전지내부에서 발생하는 모든 저항요소들을 감소시켜 더 높은 전력 밀도를 생산해야 될 필요가 있으며, 예를 들어 신진대사가 활발한 미생물의 종류, 전극의 재료 및 형태의 개선을 통해 전력밀도를 증가 시킬 수 있다. Therefore, in order to put the microbial fuel cell into practical use, it is necessary to reduce all the resistance elements generated in the cell to produce a higher power density. For example, it is necessary to improve the kind of microorganisms, The power density can be increased.

본 발명은 기존 탄소섬유를 미생물 연료전지의 전극으로 이용하는 장치의 기술을 발전시키기 위한 것으로써 탄소섬유 내 금속 촉매를 코팅하여 전력밀도향상 및 전지 내부에서 발생하는 저항요소를 감소시키는 것을 목적으로 한다. 또한 전기활성적 미생물의 성장과 군집형성을 용이하게 하고 전기전도성이 우수한 전극으로 부터 결과적으로 전력 생산 효율을 높이기 위한 새로운 전극을 개발하는데 목적이 있다.The present invention aims at developing the technology of an apparatus using an existing carbon fiber as an electrode of a microbial fuel cell and coating the metal catalyst in the carbon fiber to improve the power density and reduce the resistance element generated inside the battery. It is also intended to develop a new electrode for facilitating the growth of an electroactive microorganism and the formation of a community and for increasing the electric power production efficiency as a result of an electrode having excellent electric conductivity.

상기 목적을 달성하기 위한 본 발명은 고분자 폴리머 용액에 전기를 연결하여 표면전하의 정전기적 반발력을 이용한 nano 사이즈의 섬유를 제조하는 장치를 이용하였다.In order to achieve the above object, the present invention uses an apparatus for producing a nano-sized fiber using an electrostatic repulsive force of surface charge by connecting an electrical connection to a polymer polymer solution.

본 발명을 위해 Polacrylonitrile 5~10% 용액을 전기방사 장치에 연결하여 nano scale의 소재를 제조하고 이를 공기분위기에서 300℃ 온도로 탄화하여 탄소기반의 나노소재를 제조한 후 Pd 5~6 % 함유된 용액을 소재 표면에 고루 펴 바르고 약 12hr 건조 한 다음 300~350℃, 수소분위기에서 환원한다. 이후 Pd 0.2 ~ 0.25% 솔루션과 hidrazinde 3%용액을 소재 표면에 도포한 후 40℃를 유지 하면서 약 1hr 가량 유지하여 비표면적이 넓고 전기전달 효율이 높은 탄소기반의 미생물 연료전지 전극을 제조하는 방법에 관한 것이다.For the present invention, a nano scale material was prepared by connecting a 5 to 10% solution of Polacrylonitrile to an electrospinning device, carbonized at 300 ° C. in an air atmosphere to prepare a carbon-based nanomaterial, The solution is spread evenly over the surface of the material, dried for about 12 hours, and then reduced in a hydrogen atmosphere at 300 to 350 ° C. Then, a method of manufacturing a carbon-based microbial fuel cell electrode having a large specific surface area and high electric transfer efficiency by applying a 0.2 to 0.25% solution of Pd and a 3% solution of hydrazine to the surface of the material and maintaining the temperature at 40 ° C for about 1 hour .

상술한 바와같이, 본 발명에 따르면 비표면적이 넓은 탄소기반의 나노섬유에 금속촉매를 코팅함으로써 전기활성 미생물 부착이 쉬울 뿐만아니라 금속촉매로 하여금 전저전달 효율 증가시킴으로써 미생물 연료전지의 전력 생산 효율을 향상시킬 수 있다.As described above, according to the present invention, by coating a metal catalyst on a carbon-based nanofiber having a large specific surface area, adhesion of electroactive microorganisms is facilitated and the metal catalyst improves the power generation efficiency of the microbial fuel cell .

나노소재 표면에 금속촉매 입자가 코팅 됨으로써 미생물 연료전지 내 전력 생산 효율을 증가 시킬 수 있다.Coating of metal catalyst particles on the surface of the nanomaterial can increase the power production efficiency in the microbial fuel cell.

본 발명은 미생물 연료전지의 전력생산율을 극대화 시키기 위해 탄소기반의 나노섬유를 이용하였으며, 나노섬유의 경우 미생물 부착이 용이하고 비표면적이 넓어 저항손실에 따른 전압강하를 최소화 할 수 있는 특성이 있다. 특히 본 발명은 탄소기반 나노섬유 표면에 촉매금속을 코팅함으로써 전력밀도를 향상시킬 수 있으며 이는 산화전극 및 환원전극 적용에도 용이한 장점이 있다. The present invention uses carbon-based nanofibers to maximize the power generation rate of a microbial fuel cell. Nanofibers have a characteristic that they can easily adhere microorganisms and have a large specific surface area, thereby minimizing voltage drop due to resistance loss. In particular, the present invention can improve the power density by coating a catalytic metal on the surface of the carbon-based nanofibers, which is advantageous for application to an oxidizing electrode and a reducing electrode.

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Claims (1)

Polyactrlonitrle 5~10% wt(%) 및 DMF(Dimethylformamide)용액을 제조, 전기방사 장치를 이용하여 0.02 ml/min 용액을 공급하며, 50rpm의 colletor 회전속도와 분사거리 14cm 유지하여 소재제조, 제조된 소재를 105℃ oven에 약 12hr 이상 건조300~350℃, 수소분위기에서 약 8hr 탄화, Pd 5~6% 용액을 소재 표면에 도포 후 12hr 건조 후 일정온도 하에 Pd 0.2~0.25% 용액과 Hidrazine 3%용액을 소재표면에 도포하여 금속코팅Polyacturonitrile solution was prepared by using 5 ~ 10% wt (%) and DMF (Dimethylformamide) solution and 0.02 ml / min solution was supplied by electrospinning device. The colletor rotation speed of 50 rpm and the separation distance of 14 cm were maintained. At 105 ° C oven for about 12hrs. Carbonization and hydrogenation of Pd in a hydrogen atmosphere at 300~350 ° C for 5 ~ 6% solution is applied to the surface of the material for 12 hours. After drying for 12 hours, a Pd 0.2~0.25% solution and a hydrazine 3% solution To the surface of the material to form a metal coating
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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN111916773A (en) * 2020-06-28 2020-11-10 中南大学 Integrated PtCu/nano carbon fiber catalyst layer, preparation method thereof and application thereof in fuel cell
KR20210154548A (en) 2020-06-12 2021-12-21 조선대학교산학협력단 Anode Material for Microbial Fuel Cell, Method for Producing the Same and Microbial Fuel Cell Comprising the Anode Material
CN114709432A (en) * 2022-03-28 2022-07-05 武汉工程大学 High-efficiency microbial fuel cell integrated air cathode and preparation method and application thereof

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20210154548A (en) 2020-06-12 2021-12-21 조선대학교산학협력단 Anode Material for Microbial Fuel Cell, Method for Producing the Same and Microbial Fuel Cell Comprising the Anode Material
CN111916773A (en) * 2020-06-28 2020-11-10 中南大学 Integrated PtCu/nano carbon fiber catalyst layer, preparation method thereof and application thereof in fuel cell
CN114709432A (en) * 2022-03-28 2022-07-05 武汉工程大学 High-efficiency microbial fuel cell integrated air cathode and preparation method and application thereof

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