JP2018119181A - 還元触媒、ならびにそれを用いた化学反応装置、還元方法、および還元物生産システム - Google Patents
還元触媒、ならびにそれを用いた化学反応装置、還元方法、および還元物生産システム Download PDFInfo
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- JP2018119181A JP2018119181A JP2017011523A JP2017011523A JP2018119181A JP 2018119181 A JP2018119181 A JP 2018119181A JP 2017011523 A JP2017011523 A JP 2017011523A JP 2017011523 A JP2017011523 A JP 2017011523A JP 2018119181 A JP2018119181 A JP 2018119181A
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- XUAXVBUVQVRIIQ-UHFFFAOYSA-N 1-butyl-2,3-dimethylimidazol-3-ium Chemical compound CCCCN1C=C[N+](C)=C1C XUAXVBUVQVRIIQ-UHFFFAOYSA-N 0.000 description 1
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- IRGDPGYNHSIIJJ-UHFFFAOYSA-N 1-ethyl-2,3-dimethylimidazol-3-ium Chemical compound CCN1C=C[N+](C)=C1C IRGDPGYNHSIIJJ-UHFFFAOYSA-N 0.000 description 1
- OIDIRWZVUWCCCO-UHFFFAOYSA-N 1-ethylpyridin-1-ium Chemical compound CC[N+]1=CC=CC=C1 OIDIRWZVUWCCCO-UHFFFAOYSA-N 0.000 description 1
- BMVXCPBXGZKUPN-UHFFFAOYSA-N 1-hexanamine Chemical compound CCCCCCN BMVXCPBXGZKUPN-UHFFFAOYSA-N 0.000 description 1
- SWWLEHMBKPSRSI-UHFFFAOYSA-N 1-hexyl-2,3-dimethylimidazol-3-ium Chemical compound CCCCCCN1C=C[N+](C)=C1C SWWLEHMBKPSRSI-UHFFFAOYSA-N 0.000 description 1
- AMKUSFIBHAUBIJ-UHFFFAOYSA-N 1-hexylpyridin-1-ium Chemical compound CCCCCC[N+]1=CC=CC=C1 AMKUSFIBHAUBIJ-UHFFFAOYSA-N 0.000 description 1
- HOZSKYZXBJWURK-UHFFFAOYSA-N 1-pentylpyridin-1-ium Chemical compound CCCCC[N+]1=CC=CC=C1 HOZSKYZXBJWURK-UHFFFAOYSA-N 0.000 description 1
- CRTKBIFIDSNKCN-UHFFFAOYSA-N 1-propylpyridin-1-ium Chemical compound CCC[N+]1=CC=CC=C1 CRTKBIFIDSNKCN-UHFFFAOYSA-N 0.000 description 1
- ZVJYVLSWSYMCMF-UHFFFAOYSA-N 11-(10-carboxydecyldisulfanyl)undecanoic acid Chemical compound OC(=O)CCCCCCCCCCSSCCCCCCCCCCC(O)=O ZVJYVLSWSYMCMF-UHFFFAOYSA-N 0.000 description 1
- DIXRLQJYISYSEL-UHFFFAOYSA-N 11-aminoundecane-1-thiol Chemical compound NCCCCCCCCCCCS DIXRLQJYISYSEL-UHFFFAOYSA-N 0.000 description 1
- GWOLZNVIRIHJHB-UHFFFAOYSA-N 11-mercaptoundecanoic acid Chemical compound OC(=O)CCCCCCCCCCS GWOLZNVIRIHJHB-UHFFFAOYSA-N 0.000 description 1
- YYSCJLLOWOUSHH-UHFFFAOYSA-N 4,4'-disulfanyldibutanoic acid Chemical compound OC(=O)CCCSSCCCC(O)=O YYSCJLLOWOUSHH-UHFFFAOYSA-N 0.000 description 1
- DTRIDVOOPAQEEL-UHFFFAOYSA-N 4-sulfanylbutanoic acid Chemical compound OC(=O)CCCS DTRIDVOOPAQEEL-UHFFFAOYSA-N 0.000 description 1
- LUJDBRJEFFQGHD-UHFFFAOYSA-N 6-(5-carboxypentyldisulfanyl)hexanoic acid Chemical compound OC(=O)CCCCCSSCCCCCC(O)=O LUJDBRJEFFQGHD-UHFFFAOYSA-N 0.000 description 1
- CMNQZZPAVNBESS-UHFFFAOYSA-N 6-sulfanylhexanoic acid Chemical compound OC(=O)CCCCCS CMNQZZPAVNBESS-UHFFFAOYSA-N 0.000 description 1
- VMTVUDJOOMHKPO-UHFFFAOYSA-N 8-(7-carboxyheptyldisulfanyl)octanoic acid Chemical compound OC(=O)CCCCCCCSSCCCCCCCC(O)=O VMTVUDJOOMHKPO-UHFFFAOYSA-N 0.000 description 1
- BWUPKMHSAHUZGN-UHFFFAOYSA-N 8-aminooctane-1-thiol Chemical compound NCCCCCCCCS BWUPKMHSAHUZGN-UHFFFAOYSA-N 0.000 description 1
- FYEMIKRWWMYBFG-UHFFFAOYSA-N 8-sulfanyloctanoic acid Chemical compound OC(=O)CCCCCCCS FYEMIKRWWMYBFG-UHFFFAOYSA-N 0.000 description 1
- 229920001817 Agar Polymers 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-M Bicarbonate Chemical compound OC([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-M 0.000 description 1
- CPELXLSAUQHCOX-UHFFFAOYSA-M Bromide Chemical compound [Br-] CPELXLSAUQHCOX-UHFFFAOYSA-M 0.000 description 1
- FBFHHFIJHKHMCG-UHFFFAOYSA-N C(CCCCCCCCC)(S)S.C(CCCCCCCCCCCCCCC)(C(=O)O)C(=O)O Chemical compound C(CCCCCCCCC)(S)S.C(CCCCCCCCCCCCCCC)(C(=O)O)C(=O)O FBFHHFIJHKHMCG-UHFFFAOYSA-N 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- 229910004613 CdTe Inorganic materials 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- 229910017135 Fe—O Inorganic materials 0.000 description 1
- 229920003935 Flemion® Polymers 0.000 description 1
- 229910001218 Gallium arsenide Inorganic materials 0.000 description 1
- PQBAWAQIRZIWIV-UHFFFAOYSA-N N-methylpyridinium Chemical compound C[N+]1=CC=CC=C1 PQBAWAQIRZIWIV-UHFFFAOYSA-N 0.000 description 1
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 description 1
- URTWAZFPPIQCGS-UHFFFAOYSA-N SCCCCCCC=1NC=CN=1 Chemical compound SCCCCCCC=1NC=CN=1 URTWAZFPPIQCGS-UHFFFAOYSA-N 0.000 description 1
- 229910000577 Silicon-germanium Inorganic materials 0.000 description 1
- 229910003809 Sr-Fe Inorganic materials 0.000 description 1
- 238000005411 Van der Waals force Methods 0.000 description 1
- LEVVHYCKPQWKOP-UHFFFAOYSA-N [Si].[Ge] Chemical compound [Si].[Ge] LEVVHYCKPQWKOP-UHFFFAOYSA-N 0.000 description 1
- ITBPIKUGMIZTJR-UHFFFAOYSA-N [bis(hydroxymethyl)amino]methanol Chemical compound OCN(CO)CO ITBPIKUGMIZTJR-UHFFFAOYSA-N 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 239000008272 agar Substances 0.000 description 1
- 125000003158 alcohol group Chemical group 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- 125000001931 aliphatic group Chemical group 0.000 description 1
- 125000000217 alkyl group Chemical group 0.000 description 1
- 125000002947 alkylene group Chemical group 0.000 description 1
- 239000003011 anion exchange membrane Substances 0.000 description 1
- 239000002585 base Substances 0.000 description 1
- SLSPYQCCSCAKIB-UHFFFAOYSA-N bis(1,1,2,2,2-pentafluoroethylsulfonyl)azanide Chemical compound FC(F)(F)C(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)C(F)(F)F SLSPYQCCSCAKIB-UHFFFAOYSA-N 0.000 description 1
- SMTOKHQOVJRXLK-UHFFFAOYSA-N butane-1,4-dithiol Chemical compound SCCCCS SMTOKHQOVJRXLK-UHFFFAOYSA-N 0.000 description 1
- 150000001720 carbohydrates Chemical class 0.000 description 1
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000005341 cation exchange Methods 0.000 description 1
- 239000001913 cellulose Substances 0.000 description 1
- 229920002678 cellulose Polymers 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000007806 chemical reaction intermediate Substances 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- RAJISUUPOAJLEQ-UHFFFAOYSA-N chloromethanamine Chemical compound NCCl RAJISUUPOAJLEQ-UHFFFAOYSA-N 0.000 description 1
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 229910021419 crystalline silicon Inorganic materials 0.000 description 1
- UOQACRNTVQWTFF-UHFFFAOYSA-N decane-1,10-dithiol Chemical compound SCCCCCCCCCCS UOQACRNTVQWTFF-UHFFFAOYSA-N 0.000 description 1
- ZBCBWPMODOFKDW-UHFFFAOYSA-N diethanolamine Chemical compound OCCNCCO ZBCBWPMODOFKDW-UHFFFAOYSA-N 0.000 description 1
- HPNMFZURTQLUMO-UHFFFAOYSA-N diethylamine Chemical compound CCNCC HPNMFZURTQLUMO-UHFFFAOYSA-N 0.000 description 1
- WEHWNAOGRSTTBQ-UHFFFAOYSA-N dipropylamine Chemical compound CCCNCCC WEHWNAOGRSTTBQ-UHFFFAOYSA-N 0.000 description 1
- NVUDVUDVVXAWGV-UHFFFAOYSA-N dodecane-1,12-dithiol Chemical compound SCCCCCCCCCCCCS NVUDVUDVVXAWGV-UHFFFAOYSA-N 0.000 description 1
- 238000002296 dynamic light scattering Methods 0.000 description 1
- 238000003411 electrode reaction Methods 0.000 description 1
- 238000004453 electron probe microanalysis Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 229910052732 germanium Inorganic materials 0.000 description 1
- 229910052736 halogen Inorganic materials 0.000 description 1
- 150000002367 halogens Chemical class 0.000 description 1
- RVVRZLSZZKMJCB-UHFFFAOYSA-N heptane-1,7-dithiol Chemical compound SCCCCCCCS RVVRZLSZZKMJCB-UHFFFAOYSA-N 0.000 description 1
- 238000004128 high performance liquid chromatography Methods 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 230000002209 hydrophobic effect Effects 0.000 description 1
- 238000002329 infrared spectrum Methods 0.000 description 1
- 238000004255 ion exchange chromatography Methods 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- XMYQHJDBLRZMLW-UHFFFAOYSA-N methanolamine Chemical compound NCO XMYQHJDBLRZMLW-UHFFFAOYSA-N 0.000 description 1
- 229940087646 methanolamine Drugs 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- DIAIBWNEUYXDNL-UHFFFAOYSA-N n,n-dihexylhexan-1-amine Chemical compound CCCCCCN(CCCCCC)CCCCCC DIAIBWNEUYXDNL-UHFFFAOYSA-N 0.000 description 1
- GNVRJGIVDSQCOP-UHFFFAOYSA-N n-ethyl-n-methylethanamine Chemical compound CCN(C)CC GNVRJGIVDSQCOP-UHFFFAOYSA-N 0.000 description 1
- PXSXRABJBXYMFT-UHFFFAOYSA-N n-hexylhexan-1-amine Chemical compound CCCCCCNCCCCCC PXSXRABJBXYMFT-UHFFFAOYSA-N 0.000 description 1
- UVBMZKBIZUWTLV-UHFFFAOYSA-N n-methyl-n-propylpropan-1-amine Chemical compound CCCN(C)CCC UVBMZKBIZUWTLV-UHFFFAOYSA-N 0.000 description 1
- JACMPVXHEARCBO-UHFFFAOYSA-N n-pentylpentan-1-amine Chemical compound CCCCCNCCCCC JACMPVXHEARCBO-UHFFFAOYSA-N 0.000 description 1
- 230000003472 neutralizing effect Effects 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- KMTUBAIXCBHPIZ-UHFFFAOYSA-N pentane-1,5-dithiol Chemical compound SCCCCCS KMTUBAIXCBHPIZ-UHFFFAOYSA-N 0.000 description 1
- 229940100684 pentylamine Drugs 0.000 description 1
- 229920005597 polymer membrane Polymers 0.000 description 1
- ZJLMKPKYJBQJNH-UHFFFAOYSA-N propane-1,3-dithiol Chemical compound SCCCS ZJLMKPKYJBQJNH-UHFFFAOYSA-N 0.000 description 1
- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 description 1
- 238000004445 quantitative analysis Methods 0.000 description 1
- 238000001028 reflection method Methods 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 238000012764 semi-quantitative analysis Methods 0.000 description 1
- 230000035945 sensitivity Effects 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 238000004611 spectroscopical analysis Methods 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 125000001424 substituent group Chemical group 0.000 description 1
- 125000004434 sulfur atom Chemical group 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- VRMLAAZCMTWSHJ-UHFFFAOYSA-N tetradecane-1,14-dithiol Chemical compound SCCCCCCCCCCCCCCS VRMLAAZCMTWSHJ-UHFFFAOYSA-N 0.000 description 1
- 150000003573 thiols Chemical group 0.000 description 1
- 238000006276 transfer reaction Methods 0.000 description 1
- 239000012780 transparent material Substances 0.000 description 1
- IMFACGCPASFAPR-UHFFFAOYSA-N tributylamine Chemical compound CCCCN(CCCC)CCCC IMFACGCPASFAPR-UHFFFAOYSA-N 0.000 description 1
- CITYNMLIOBJLMN-UHFFFAOYSA-N tridecane-1,13-dithiol Chemical compound SCCCCCCCCCCCCCS CITYNMLIOBJLMN-UHFFFAOYSA-N 0.000 description 1
- YFTHZRPMJXBUME-UHFFFAOYSA-N tripropylamine Chemical compound CCCN(CCC)CCC YFTHZRPMJXBUME-UHFFFAOYSA-N 0.000 description 1
- 230000005641 tunneling Effects 0.000 description 1
- 238000004704 ultra performance liquid chromatography Methods 0.000 description 1
- CCIDWXHLGNEQSL-UHFFFAOYSA-N undecane-1-thiol Chemical compound CCCCCCCCCCCS CCIDWXHLGNEQSL-UHFFFAOYSA-N 0.000 description 1
- 239000003643 water by type Substances 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
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Abstract
Description
Raはそれぞれ独立にHまたはC1〜C4アルキル基であり、
Zは、窒素原子を2つ以上含む芳香族環であり、
Yは、前記導電層と結合し得るヘテロ原子含有基であり、
naは、1以上5以下の整数であり、
nbは0以上6以下の整数である)
で表される構造を有することを特徴とするものである。
酸化電極と、
前記還元触媒を具備する還元電極と、
前記酸化電極及び前記還元電極に接続された電源ユニットと、
を具備することを特徴とするものである。
前記還元触媒を含む還元電極を電解液に接触させる工程と、
前記電解液に低分子炭素化合物を導入し、導入された前記低分子炭素化合物を前記電極によって還元する工程と、
を含むことを特徴とするものである。
酸化触媒を備えた酸化反応用電解槽、および
前記還元触媒を備えた還元反応用電解槽
を備え、二酸化炭素を還元して還元物を生成する化学反応装置と、
前記還元反応用電解槽に電解液を供給する電解液供給ユニットと、
前記電解液に二酸化炭素を溶解させて前記還元反応用電解槽における還元反応を持続させることにより、前記電解液中の前記還元物の濃度を上昇させる二酸化炭素供給ユニットと、
前記還元物の濃度が上昇した電解液から前記還元物を分離する分離ユニットと、
を備えることを特徴とするものである。
第1実施形態に係る還元触媒は導電体と、前記導電体の表面に修飾有機基からなる有機層を備えるものである。
Raはそれぞれ独立にHまたはC1〜C4アルキル基であり、
Zは、窒素原子を2つ以上含む芳香族環であり、
Yは、前記導電層と結合し得るヘテロ原子含有基であり、
naは、1以上5以下の整数であり、
nbは0以上6以下の整数である)
で表される構造を有するものを用いることができる。これらの修飾有機基は、naまたはnbが比較的短いために、還元反応の起こる場所が導電体に近くなるので、高い反応効率が実現できるものと考えられる。
まず、集電体101の表面に導電体102を形成する。その方法としては、スパッタ法、蒸着法、またはALD(Atomic Layer Deposition)法等の既知の真空成膜方法を用いることができる。
図2は、本実施形態に係る還元触媒150の構成を示す図である。図2に示すように、還元触媒150は、導電体102を有する集電体101と、導電体102の表面に形成されたスペーサー有機分子層105と、スペーサー有機分子層105の表面に結合された金属微粒子107と、金属微粒子107に結合された修飾有機基112とを備える。
第3実施形態では、第1実施形態に係る還元触媒を用いた化学反応装置について説明する。なお、記載を省略するが、第1実施形態に係る還元触媒の代わりに、第2実施形態に係る還元触媒を用いることも可能である。
2H2O → 4H++O2+4e− ・・・(1)
2CO2+4H++4e− → 2CO+2H2O ・・・(2)
4OH− → O2+2H2O+4e− ・・・(3)
2CO2+2H2O+4e− → 2CO+4OH− ・・・(4)
修飾有機基112の結合状態と分子密度は、X線光電子分光法(XPS)による分析結果に基づいて算出できる。分析条件は、以下の条件とすることができる。なお、検出角度とは、試料法線と検出器入力レンズ軸の成す角を示している。
使用機種 PHI社製 Quantera-SXM
照射X線源 単結晶分光AlKα線
出力 50W
分析領域 φ200μm
Pass Energy Wide Scan-280.0eV(1.0eV/Step)
Narrow Scan-69.0eV(0.125eV/Step)
検出角度 45°
帯電中和電子銃 Ar+,e−共に使用
単位あたりAu原子数(atoms/cm2)
=密度(g/cm3)×検出深さ(nm)×N/Mw ・・・(5)
分子密度(atoms/cm2)
=Au(atoms/cm2)×S/Au(原子数比) ・・・(6)
以上のように、本実施形態によれば、反応効率の高い化学反応装置を提供することができる。
基材表面(金属層)をAuにより構成し、修飾有機分子としてアミノエタンチオールを用いて、実施例1の還元触媒を作製した。
修飾有機分子として表2に記載した化合物を用いた以外は、実施例1と同様に実施例2の還元触媒を作製した。
修飾有機分子を用いなかった以外は、実施例1と同様に比較例1の還元触媒を作製した。
修飾有機分子として表2に記載した化合物を用いた以外は、実施例1と同様に実施例2の還元触媒を作製した。ここで用いた修飾有機分子は、式(A)のnaが実施形態の範囲外であるものであった。
金属層を、表2に記載した材料により構成した以外は、実施例1と同様に実施例16〜25の還元触媒を作製した。
金属層を、表2に記載した材料により構成し、修飾有機分子を用いなかった以外は、実施例1と同様に比較例3〜13の還元触媒を作製した。
実施例1〜25及び比較例1〜13における還元触媒を用いて三電極式セルを作製した。
基材表面(金属層)をAuにより構成し、スペーサー有機分子及び修飾有機分子としてメルカプトエチルイミダゾールを用い、金属微粒子として平均粒子径が3nmのAu粒子を用いて、実施例26の還元触媒を作製した。なお、金属微粒子の平均粒子径は、粒度分布計(ゼータサイザーナノZS、マルバーン製)を用いて測定した。
電解液として、トリエタノールアミン水溶液(50wt%水溶液、CO2飽和吸収液)を用いた以外は、実施例26と同様に三電極式セルを作製した。
電解液として、90%1−エチル−3−メチルイミダゾリウムテトラフルオロボラート水溶液(EMIBF4、CO2飽和吸収液)を用いた以外は、実施例26と同様に三電極式セルを作製した。
比較例1と同様に、スペーサー有機分子、金属微粒子、及び修飾有機分子を有さない還元触媒を作製した。この還元触媒を用い、電解液として、トリエタノールアミン水溶液(50wt%水溶液、CO2飽和吸収液)を用いた以外は、実施例26と同様に三電極式セルを作製した。
比較例1と同様に、スペーサー有機分子、金属微粒子、及び修飾有機分子を有さない還元触媒を作製した。この還元触媒を用い、電解液として、90%1−エチル−3−メチルイミダゾリウムテトラフルオロボラート水溶液(EMIBF4、CO2飽和吸収液)を用いた以外は、実施例26と同様に三電極式セルを作製した。
実施例26〜28及び比較例15〜16のそれぞれの三電極式セルについて、CO2還元性能を上記の方法と同様に評価した。その結果を表3に示す。なお、参考のため、表3には比較例1の結果も示した。
多接合型太陽電池の基板を集電体として用い、スペーサー有機分子及び修飾有機分子としてメルカプトエチルトリアゾールを用いた以外は、実施例26と同様に還元触媒を作製した。この多接合型太陽電池の酸化電極層の表面に、酸化触媒層を形成した。具体的には、酸化ニッケルのナノ粒子をアルコール水溶液に分散した分散液を、酸化電極層の表面にスプレー塗布法により塗布した。このようにして、実施例26の光化学反応セルを作製し、150mm×250mmの大きさに切りだした。
多接合型太陽電池の基板を集電体として用い、比較例1と同様に、スペーサー有機分子、金属微粒子、及び修飾有機分子のいずれも含有しない還元触媒を作製した。この多接合型太陽電池の酸化電極層の表面に、酸化触媒層を形成した。具体的には、酸化ニッケルのナノ粒子をアルコール水溶液に分散した分散液を、酸化電極層の表面にスプレー塗布法により塗布した。このようにして比較例15の光化学反応セルを作製し、150mm×250mmの大きさに切りだした。
実施例29及び比較例17の光化学反応セルを化学反応装置に組み込み、エネルギー変換効率を評価した。酸化側電解液として、0.5M水酸化カリウム(KOH)水溶液を用い、還元側電解液として、トリエタノールアミン水溶液(50wt%水溶液、CO2飽和吸収液)を用いた。また、イオン交換膜としてプロトン交換膜を用いた。酸化触媒層側からソーラーシュミレータによるAM1.5(100mW/cm2)の光を照射し、還元側で発生するCOガスをガスクロマトグラフィーで全てのCO2還元物について実施例1と同様に定量分析した。その結果に基づいてエネルギー変換効率を算出した。エネルギー変換効率は下記(7)式によって算出した。
FE/SE ×100 (7)
(7)式において、SEは照射された太陽光エネルギーを示し、FEは生成された物質のもつギブス自由エネルギーを示す。測定結果を表4に示す。
Claims (13)
- 前記Yが、メルカプト基である、請求項1に記載の還元触媒。
- 前記Zが、イミダゾール基またはトリアゾール基である、請求項1または2に記載の還元触媒。
- 前記有修飾基が、アミノエタンチオール、アミノプロパンチオール、アミノブタンチオール、メチルアミノエタンチオール、イソプロピルエチルアミノエタンチオール、ジメチルアミノエタンチオール、ジエチルアミノエタンチオール、ジブチルアミノエタンチオール、メルカプトエチルイミダゾール、メルカプトプロピルイミダゾール、メルカプトブチルイミダゾール、カプトヘキシルイミダゾール、メルカプトトリアゾール、メルカプトエチルトリアゾール、メルカプトプロピルトリアゾール、メルカプトブチルトリアゾール、およびメルカプトヘキシルトリアゾールからなる群から選択される有機化合物から誘導される基である、請求項1〜3のいずれか1項に記載の還元触媒。
- 前記導電体が、Au、Ag、Cu、Pt、Pd、Zn、Fe、Ti、Sn、In、Hg、BiおよびNiからなる群から選択される金属を含む、請求項1〜4のいずれか1項に記載の還元触媒。
- 前記導電体が金属微粒子であり、前記金属粒子が導電性基材表面に形成された有機物からなるスペーサー層に担持されている、請求項1〜5のいずれか1項に記載の還元触媒。
- 前記導電体が、Ag2O、CuO、Ta2O5、TiO2、ZrO2、Al2O3、SiO2、ZnO、ITO、およびFTOからなる群から選択される酸化物を含む、請求項1〜4のいずれか1項に記載の還元触媒。
- 酸化電極と、
請求項1〜7の何れか一項に記載の還元触媒を具備する還元電極と、
前記酸化電極及び前記還元電極に接続された電源ユニットと、
を具備することを特徴とする化学反応装置。
- 前記電源ユニットが、光エネルギーにより電荷分離する半導体層を備えた、請求項8に記載の化学反応装置。
- 前記半導体層が、前記酸化電極と前記還元電極との間に配置された、請求項7に記載の化学反応装置。
- 請求項1〜7のいずれか1項に記載の還元触媒を含む還元電極を電解液に接触させる工程と、
前記電解液に低分子炭素化合物を導入し、導入された前記低分子炭素化合物を前記電極によって還元する工程と、
を含むことを特徴とする、還元方法。 - 前記低分子炭素化合物が、二酸化炭素、シュウ酸、グリオキサールからなる群から選択される、請求項11に記載に還元方法。
- 酸化触媒を備えた酸化反応用電解槽、および
請求項1〜7のいずれか一項に記載の還元触媒を備えた還元反応用電解槽
を備え、二酸化炭素を還元して還元物を生成する化学反応装置と、
前記還元反応用電解槽に電解液を供給する電解液供給ユニットと、
前記電解液に二酸化炭素を溶解させて前記還元反応用電解槽における還元反応を持続させることにより、前記電解液中の前記還元物の濃度を上昇させる二酸化炭素供給ユニットと、
前記還元物の濃度が上昇した電解液から前記還元物を分離する分離ユニットと、
を備えることを特徴とする、還元物生産システム。
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JP2022116956A (ja) * | 2021-01-29 | 2022-08-10 | 株式会社豊田中央研究所 | 還元反応用電極 |
JP7327422B2 (ja) | 2021-01-29 | 2023-08-16 | 株式会社豊田中央研究所 | 還元反応用電極 |
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