JP2010064066A - 光触媒体及びそれを用いた還元用触媒体 - Google Patents
光触媒体及びそれを用いた還元用触媒体 Download PDFInfo
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- JP2010064066A JP2010064066A JP2009184051A JP2009184051A JP2010064066A JP 2010064066 A JP2010064066 A JP 2010064066A JP 2009184051 A JP2009184051 A JP 2009184051A JP 2009184051 A JP2009184051 A JP 2009184051A JP 2010064066 A JP2010064066 A JP 2010064066A
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- Prior art keywords
- semiconductor
- photocatalyst
- base material
- complex
- light
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
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- 239000011941 photocatalyst Substances 0.000 title claims abstract description 36
- 239000003054 catalyst Substances 0.000 title claims abstract description 30
- 230000009467 reduction Effects 0.000 title description 4
- 239000004065 semiconductor Substances 0.000 claims abstract description 76
- 239000000463 material Substances 0.000 claims abstract description 40
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims abstract description 26
- 229910052702 rhenium Inorganic materials 0.000 claims abstract description 19
- WUAPFZMCVAUBPE-UHFFFAOYSA-N rhenium atom Chemical compound [Re] WUAPFZMCVAUBPE-UHFFFAOYSA-N 0.000 claims abstract description 19
- 229910052984 zinc sulfide Inorganic materials 0.000 claims abstract description 19
- 239000005083 Zinc sulfide Substances 0.000 claims abstract description 18
- DRDVZXDWVBGGMH-UHFFFAOYSA-N zinc;sulfide Chemical compound [S-2].[Zn+2] DRDVZXDWVBGGMH-UHFFFAOYSA-N 0.000 claims abstract description 18
- 238000006243 chemical reaction Methods 0.000 claims abstract description 17
- BPUBBGLMJRNUCC-UHFFFAOYSA-N oxygen(2-);tantalum(5+) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ta+5].[Ta+5] BPUBBGLMJRNUCC-UHFFFAOYSA-N 0.000 claims abstract description 16
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 13
- 229910001936 tantalum oxide Inorganic materials 0.000 claims abstract description 13
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims abstract description 11
- 229910052802 copper Inorganic materials 0.000 claims abstract description 11
- 239000010949 copper Substances 0.000 claims abstract description 11
- 230000001678 irradiating effect Effects 0.000 claims abstract description 10
- 238000006722 reduction reaction Methods 0.000 claims abstract description 9
- 229910052715 tantalum Inorganic materials 0.000 claims abstract description 6
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims abstract description 6
- MZLGASXMSKOWSE-UHFFFAOYSA-N tantalum nitride Chemical compound [Ta]#N MZLGASXMSKOWSE-UHFFFAOYSA-N 0.000 claims abstract description 6
- 239000012327 Ruthenium complex Substances 0.000 claims abstract description 4
- 150000004696 coordination complex Chemical class 0.000 claims description 20
- 239000000758 substrate Substances 0.000 claims description 17
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 claims description 8
- 238000006555 catalytic reaction Methods 0.000 claims description 7
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical compound [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 claims description 5
- 239000005751 Copper oxide Substances 0.000 claims description 5
- 229910005540 GaP Inorganic materials 0.000 claims description 5
- 229910000431 copper oxide Inorganic materials 0.000 claims description 5
- 150000001875 compounds Chemical class 0.000 claims description 4
- HZXMRANICFIONG-UHFFFAOYSA-N gallium phosphide Chemical compound [Ga]#P HZXMRANICFIONG-UHFFFAOYSA-N 0.000 claims description 4
- 238000004776 molecular orbital Methods 0.000 claims description 4
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims description 4
- 229910010271 silicon carbide Inorganic materials 0.000 claims description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 3
- GPXJNWSHGFTCBW-UHFFFAOYSA-N Indium phosphide Chemical compound [In]#P GPXJNWSHGFTCBW-UHFFFAOYSA-N 0.000 claims description 3
- 229910052799 carbon Inorganic materials 0.000 claims description 3
- 230000005284 excitation Effects 0.000 claims 1
- 230000001747 exhibiting effect Effects 0.000 claims 1
- ROFVEXUMMXZLPA-UHFFFAOYSA-N Bipyridyl Chemical compound N1=CC=CC=C1C1=CC=CC=N1 ROFVEXUMMXZLPA-UHFFFAOYSA-N 0.000 abstract description 38
- 239000003446 ligand Substances 0.000 abstract description 12
- -1 carboxy bipyridine Chemical compound 0.000 abstract description 3
- 239000002253 acid Substances 0.000 abstract 1
- 150000004767 nitrides Chemical class 0.000 abstract 1
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 description 43
- 230000000052 comparative effect Effects 0.000 description 38
- 239000000843 powder Substances 0.000 description 32
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 26
- 239000007789 gas Substances 0.000 description 26
- 239000000243 solution Substances 0.000 description 26
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 24
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 24
- 229910002091 carbon monoxide Inorganic materials 0.000 description 24
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 22
- 235000019253 formic acid Nutrition 0.000 description 22
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 21
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 description 21
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 16
- 239000001569 carbon dioxide Substances 0.000 description 13
- 229910002092 carbon dioxide Inorganic materials 0.000 description 13
- 229920001971 elastomer Polymers 0.000 description 13
- GSEJCLTVZPLZKY-UHFFFAOYSA-N Triethanolamine Chemical compound OCCN(CCO)CCO GSEJCLTVZPLZKY-UHFFFAOYSA-N 0.000 description 12
- 229910052786 argon Inorganic materials 0.000 description 11
- 238000004519 manufacturing process Methods 0.000 description 11
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 10
- 229910052739 hydrogen Inorganic materials 0.000 description 10
- 239000001257 hydrogen Substances 0.000 description 10
- 238000004768 lowest unoccupied molecular orbital Methods 0.000 description 10
- 239000000047 product Substances 0.000 description 10
- 229910021529 ammonia Inorganic materials 0.000 description 7
- 229920006395 saturated elastomer Polymers 0.000 description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 7
- OQVVVVYHNKQXHR-UHFFFAOYSA-N 2-pyridin-2-ylpyridine-3-carboxylic acid Chemical compound OC(=O)C1=CC=CN=C1C1=CC=CC=N1 OQVVVVYHNKQXHR-UHFFFAOYSA-N 0.000 description 6
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 6
- 229910052751 metal Inorganic materials 0.000 description 6
- 239000000126 substance Substances 0.000 description 6
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 5
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 5
- 239000013078 crystal Substances 0.000 description 5
- 238000005259 measurement Methods 0.000 description 5
- 239000002184 metal Substances 0.000 description 5
- 239000012071 phase Substances 0.000 description 5
- 239000011701 zinc Substances 0.000 description 5
- 229910052725 zinc Inorganic materials 0.000 description 5
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 4
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 4
- 238000002441 X-ray diffraction Methods 0.000 description 4
- 230000008859 change Effects 0.000 description 4
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Chemical compound [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 238000005304 joining Methods 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- 239000006228 supernatant Substances 0.000 description 4
- JIAARYAFYJHUJI-UHFFFAOYSA-L zinc dichloride Chemical compound [Cl-].[Cl-].[Zn+2] JIAARYAFYJHUJI-UHFFFAOYSA-L 0.000 description 4
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 3
- 239000007864 aqueous solution Substances 0.000 description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- KBJMLQFLOWQJNF-UHFFFAOYSA-N nickel(ii) nitrate Chemical compound [Ni+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O KBJMLQFLOWQJNF-UHFFFAOYSA-N 0.000 description 3
- 239000003960 organic solvent Substances 0.000 description 3
- 229910052760 oxygen Inorganic materials 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 229910052707 ruthenium Inorganic materials 0.000 description 3
- 239000002904 solvent Substances 0.000 description 3
- 238000003756 stirring Methods 0.000 description 3
- PBCFLUZVCVVTBY-UHFFFAOYSA-N tantalum pentoxide Inorganic materials O=[Ta](=O)O[Ta](=O)=O PBCFLUZVCVVTBY-UHFFFAOYSA-N 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 3
- JGPSMWXKRPZZRG-UHFFFAOYSA-N zinc;dinitrate;hexahydrate Chemical compound O.O.O.O.O.O.[Zn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O JGPSMWXKRPZZRG-UHFFFAOYSA-N 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 2
- 229910003071 TaON Inorganic materials 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 2
- ZOIORXHNWRGPMV-UHFFFAOYSA-N acetic acid;zinc Chemical compound [Zn].CC(O)=O.CC(O)=O ZOIORXHNWRGPMV-UHFFFAOYSA-N 0.000 description 2
- 230000009471 action Effects 0.000 description 2
- 239000012298 atmosphere Substances 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 239000007795 chemical reaction product Substances 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- 239000012153 distilled water Substances 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- 238000011156 evaluation Methods 0.000 description 2
- 239000010408 film Substances 0.000 description 2
- 238000010438 heat treatment Methods 0.000 description 2
- 150000004687 hexahydrates Chemical class 0.000 description 2
- 239000012535 impurity Substances 0.000 description 2
- 229910021645 metal ion Inorganic materials 0.000 description 2
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 description 2
- 239000011259 mixed solution Substances 0.000 description 2
- 238000002156 mixing Methods 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 239000004570 mortar (masonry) Substances 0.000 description 2
- 238000013032 photocatalytic reaction Methods 0.000 description 2
- 229940048181 sodium sulfide nonahydrate Drugs 0.000 description 2
- WMDLZMCDBSJMTM-UHFFFAOYSA-M sodium;sulfanide;nonahydrate Chemical compound O.O.O.O.O.O.O.O.O.[Na+].[SH-] WMDLZMCDBSJMTM-UHFFFAOYSA-M 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 239000000725 suspension Substances 0.000 description 2
- OEIMLTQPLAGXMX-UHFFFAOYSA-I tantalum(v) chloride Chemical compound Cl[Ta](Cl)(Cl)(Cl)Cl OEIMLTQPLAGXMX-UHFFFAOYSA-I 0.000 description 2
- 230000036962 time dependent Effects 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- 230000007306 turnover Effects 0.000 description 2
- 229910052724 xenon Inorganic materials 0.000 description 2
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 2
- 239000004246 zinc acetate Substances 0.000 description 2
- 239000011592 zinc chloride Substances 0.000 description 2
- 235000005074 zinc chloride Nutrition 0.000 description 2
- ONDPHDOFVYQSGI-UHFFFAOYSA-N zinc nitrate Chemical compound [Zn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ONDPHDOFVYQSGI-UHFFFAOYSA-N 0.000 description 2
- NWONKYPBYAMBJT-UHFFFAOYSA-L zinc sulfate Chemical compound [Zn+2].[O-]S([O-])(=O)=O NWONKYPBYAMBJT-UHFFFAOYSA-L 0.000 description 2
- 229910000368 zinc sulfate Inorganic materials 0.000 description 2
- 229960001763 zinc sulfate Drugs 0.000 description 2
- RXBXBWBHKPGHIB-UHFFFAOYSA-L zinc;diperchlorate Chemical compound [Zn+2].[O-]Cl(=O)(=O)=O.[O-]Cl(=O)(=O)=O RXBXBWBHKPGHIB-UHFFFAOYSA-L 0.000 description 2
- ZFYIQPIHXRFFCZ-QMMMGPOBSA-N (2s)-2-(cyclohexylamino)butanedioic acid Chemical compound OC(=O)C[C@@H](C(O)=O)NC1CCCCC1 ZFYIQPIHXRFFCZ-QMMMGPOBSA-N 0.000 description 1
- 238000001644 13C nuclear magnetic resonance spectroscopy Methods 0.000 description 1
- UTXZJSXPLRXPKU-UHFFFAOYSA-N 2-pyridin-2-ylpyridine-3,4-dicarboxylic acid Chemical group OC(=O)C1=CC=NC(C=2N=CC=CC=2)=C1C(O)=O UTXZJSXPLRXPKU-UHFFFAOYSA-N 0.000 description 1
- 125000004105 2-pyridyl group Chemical group N1=C([*])C([H])=C([H])C([H])=C1[H] 0.000 description 1
- 229910021586 Nickel(II) chloride Inorganic materials 0.000 description 1
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 1
- MQRWBMAEBQOWAF-UHFFFAOYSA-N acetic acid;nickel Chemical compound [Ni].CC(O)=O.CC(O)=O MQRWBMAEBQOWAF-UHFFFAOYSA-N 0.000 description 1
- 150000001412 amines Chemical class 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- SMWDFEZZVXVKRB-UHFFFAOYSA-N anhydrous quinoline Natural products N1=CC=CC2=CC=CC=C21 SMWDFEZZVXVKRB-UHFFFAOYSA-N 0.000 description 1
- 125000005605 benzo group Chemical group 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000012159 carrier gas Substances 0.000 description 1
- 239000007806 chemical reaction intermediate Substances 0.000 description 1
- 239000012141 concentrate Substances 0.000 description 1
- 238000011109 contamination Methods 0.000 description 1
- 229910000365 copper sulfate Inorganic materials 0.000 description 1
- ORTQZVOHEJQUHG-UHFFFAOYSA-L copper(II) chloride Chemical compound Cl[Cu]Cl ORTQZVOHEJQUHG-UHFFFAOYSA-L 0.000 description 1
- ARUVKPQLZAKDPS-UHFFFAOYSA-L copper(II) sulfate Chemical compound [Cu+2].[O-][S+2]([O-])([O-])[O-] ARUVKPQLZAKDPS-UHFFFAOYSA-L 0.000 description 1
- OPQARKPSCNTWTJ-UHFFFAOYSA-L copper(ii) acetate Chemical compound [Cu+2].CC([O-])=O.CC([O-])=O OPQARKPSCNTWTJ-UHFFFAOYSA-L 0.000 description 1
- YRNNKGFMTBWUGL-UHFFFAOYSA-L copper(ii) perchlorate Chemical compound [Cu+2].[O-]Cl(=O)(=O)=O.[O-]Cl(=O)(=O)=O YRNNKGFMTBWUGL-UHFFFAOYSA-L 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- XNFVGEUMTFIVHQ-UHFFFAOYSA-N disodium;sulfide;hydrate Chemical compound O.[Na+].[Na+].[S-2] XNFVGEUMTFIVHQ-UHFFFAOYSA-N 0.000 description 1
- 238000002848 electrochemical method Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000004817 gas chromatography Methods 0.000 description 1
- 239000001307 helium Substances 0.000 description 1
- 229910052734 helium Inorganic materials 0.000 description 1
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 description 1
- 238000004770 highest occupied molecular orbital Methods 0.000 description 1
- 230000007062 hydrolysis Effects 0.000 description 1
- 238000006460 hydrolysis reaction Methods 0.000 description 1
- 238000004255 ion exchange chromatography Methods 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 230000031700 light absorption Effects 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
- 229910052753 mercury Inorganic materials 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 125000000896 monocarboxylic acid group Chemical group 0.000 description 1
- 229940078494 nickel acetate Drugs 0.000 description 1
- QMMRZOWCJAIUJA-UHFFFAOYSA-L nickel dichloride Chemical compound Cl[Ni]Cl QMMRZOWCJAIUJA-UHFFFAOYSA-L 0.000 description 1
- LGQLOGILCSXPEA-UHFFFAOYSA-L nickel sulfate Chemical compound [Ni+2].[O-]S([O-])(=O)=O LGQLOGILCSXPEA-UHFFFAOYSA-L 0.000 description 1
- AOPCKOPZYFFEDA-UHFFFAOYSA-N nickel(2+);dinitrate;hexahydrate Chemical compound O.O.O.O.O.O.[Ni+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O AOPCKOPZYFFEDA-UHFFFAOYSA-N 0.000 description 1
- ZLQBNKOPBDZKDP-UHFFFAOYSA-L nickel(2+);diperchlorate Chemical compound [Ni+2].[O-]Cl(=O)(=O)=O.[O-]Cl(=O)(=O)=O ZLQBNKOPBDZKDP-UHFFFAOYSA-L 0.000 description 1
- 229910000363 nickel(II) sulfate Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 230000001699 photocatalysis Effects 0.000 description 1
- 230000001443 photoexcitation Effects 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- 125000002943 quinolinyl group Chemical group N1=C(C=CC2=CC=CC=C12)* 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 238000011946 reduction process Methods 0.000 description 1
- 230000027756 respiratory electron transport chain Effects 0.000 description 1
- 150000003303 ruthenium Chemical class 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 235000011121 sodium hydroxide Nutrition 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 238000000411 transmission spectrum Methods 0.000 description 1
- FOSPKRPCLFRZTR-UHFFFAOYSA-N zinc;dinitrate;hydrate Chemical compound O.[Zn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O FOSPKRPCLFRZTR-UHFFFAOYSA-N 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
Images
Classifications
-
- B01J35/39—
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/20—Vanadium, niobium or tantalum
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2531/00—Additional information regarding catalytic systems classified in B01J31/00
- B01J2531/70—Complexes comprising metals of Group VII (VIIB) as the central metal
- B01J2531/74—Rhenium
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2531/00—Additional information regarding catalytic systems classified in B01J31/00
- B01J2531/80—Complexes comprising metals of Group VIII as the central metal
- B01J2531/82—Metals of the platinum group
- B01J2531/821—Ruthenium
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/02—Sulfur, selenium or tellurium; Compounds thereof
- B01J27/04—Sulfides
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/16—Catalysts comprising hydrides, coordination complexes or organic compounds containing coordination complexes
- B01J31/18—Catalysts comprising hydrides, coordination complexes or organic compounds containing coordination complexes containing nitrogen, phosphorus, arsenic or antimony as complexing atoms, e.g. in pyridine ligands, or in resonance therewith, e.g. in isocyanide ligands C=N-R or as complexed central atoms
- B01J31/1805—Catalysts comprising hydrides, coordination complexes or organic compounds containing coordination complexes containing nitrogen, phosphorus, arsenic or antimony as complexing atoms, e.g. in pyridine ligands, or in resonance therewith, e.g. in isocyanide ligands C=N-R or as complexed central atoms the ligands containing nitrogen
- B01J31/181—Cyclic ligands, including e.g. non-condensed polycyclic ligands, comprising at least one complexing nitrogen atom as ring member, e.g. pyridine
- B01J31/1815—Cyclic ligands, including e.g. non-condensed polycyclic ligands, comprising at least one complexing nitrogen atom as ring member, e.g. pyridine with more than one complexing nitrogen atom, e.g. bipyridyl, 2-aminopyridine
Abstract
【解決手段】ニッケル含有硫化亜鉛、銅含有硫化亜鉛、窒化タンタル、酸窒化タンタル、酸化タンタルの少なくとも1つを含む半導体と、カルボキシビピリジン配位子を有するレニウム錯体またはビピリジン配位子を有するルテニウム錯体からなる基材と、が接合された構造を有し、半導体に光を照射することによって生じた励起電子が基材に移動することにより基材が触媒反応を呈するようにする。
【選択図】図1
Description
硝酸亜鉛(II)六水和物と硝酸ニッケル(II)六水和物を蒸留水に溶解させ、その後に硫化ナトリウム九水和物を溶解させた水溶液を投入して2時間撹拌した。このとき、溶液中の全金属イオン濃度は0.1mol/Lと一定にし、ニッケルの割合は全金属濃度に対して0.1wt%とした。撹拌後の懸濁液は遠心分離と再分散を3回繰り返し、上澄みを除去後、真空乾燥させ、得られた固体を乳鉢で粉砕してニッケル含有硫化亜鉛の半導体粉末を得た。X線回折装置(RINT−TTR,リガク)によるX線回折測定の結果、この粉末中にZnSの結晶相のみが存在することが確認された。また、分光光度計(UV−3600・ISR−3100,島津製作所)による拡散反射測定の結果、粉末は550nm以下の波長の光を吸収することが確認された。
硝酸亜鉛(II)六水和物と硝酸銅(II)三水和物を蒸留水に溶解させ、その後に硫化ナトリウム九水和物を投入して2時間撹拌した。このとき、溶液中の全金属イオン濃度は0.1mol/Lと一定にし、銅の割合は全金属濃度に対して4.5wt%とした。撹拌後の懸濁液は遠心分離と再分散を3回繰り返し、上澄みを除去後、真空乾燥させ、得られた固体を乳鉢で粉砕して銅含有硫化亜鉛の半導体粉末を得た。
酸化タンタル(V)(和光純薬工業製)をアンモニアとアルゴンをそれぞれ250sccmの流量で混合したガス流中において750℃で12時間処理し、オレンジ色の粉末を得た。X線回折測定の結果、この粉末中にはTa3N5、TaON、Ta2O5の結晶相が混在することが確認された。この粉末は620nm以下の波長の光を吸収することが分光光度計による測定で確認された。この粉末500mgとカルボキシビピリジン配位子を有するレニウム錯体((Re(dcbpy)(CO)3MeCN))2mgをメタノール中で12時間撹拌し、真空乾燥させることにより半導体と金属錯体を接合した触媒を合成した。
酸化タンタル(V)(和光純薬工業製)をアンモニアとアルゴンをそれぞれ250sccmの流量で混合したガス流中において800℃で6時間処理し、黄色の粉末を得た。X線回折測定の結果、この粉末中にはTaONの結晶相のみが存在することが確認された。この粉末は550nm以下の波長の光を吸収することが分光光度計による測定で確認された。この粉末500mgとカルボキシビピリジン配位子を有するレニウム錯体((Re(dcbpy)(CO)3MeCN))2mgをメタノール中で12時間撹拌し、真空乾燥させることにより半導体と金属錯体を接合した触媒を合成した。
酸化タンタル(V)(和光純薬工業製)3gを、透明石英管製の処理炉を用いて、アンモニアとアルゴンをそれぞれ250sccmの流量で混合したガス流中において820℃で18時間処理することにより、赤色の粉末を得た。X線回折測定の結果、この粉末中にはTa3N5の結晶相のみが存在することが確認された。この粉末は620nm以下の波長の光を吸収することが分光光度計による測定で確認された。この粉末500mgとカルボキシビピリジン配位子を有するレニウム錯体((Re(dcbpy)(CO)3MeCN))1mgをメタノール中で12時間撹拌し、真空乾燥させることにより半導体と金属錯体を接合した触媒を合成した。
実施例1におけるニッケル含有硫化亜鉛の半導体粉末を比較例1とした。
実施例3における窒化タンタル(V)の半導体粉末を比較例2とした。
実施例1から5におけるレニウム錯体((Re(dcbpy)(CO)3MeCN))を比較例3とした。
市販の酸化チタン(石原産業製、品番 ST−01)をアンモニアガス中において575℃で3時間熱処理することにより、窒素ドープ酸化チタンを作製した。この粉末はアナターゼ型結晶を有しており、また、550nm以下の光を吸収できることが確認された。この粉末500mgに比較例3のレニウム錯体4mgを、実施例5と同様の方法で吸着させたものを比較例4とした。
実施例1〜5及び比較例1〜4について光触媒体としての性能を評価した。試験管にジメチルフォルムアミドとトリエタノールアミンを合計5mL、体積比にして40:1の比で入れ、さらに実施例1〜5及び比較例1〜4で得られた物質を2mg入れた溶液をそれぞれ作成した。
5gの塩化タンタル(和光純薬)を100mLのエタノール中に溶解させ、5%のNH3水溶液を加えて300mLにメスアップし、5時間撹拌してタンタル酸化物の粉末を作成した。この白色粉末を大気中に置いて800℃で5時間熱処理した後、アンモニア(NH3)ガスを0.4L/min、アルゴン(Ar)ガスを0.2mL/minで混合流通させた条件下において575℃で5時間処理し、黄色の窒素ドープ酸化タンタル(NドープTa2O5)の粉末を作成した。8mLサイズの試験管に、アセトニトリルと電子供与剤としてトリエタノールアミン(TEOA)を5:1の体積比で混合した溶液を4mL入れ、さらにNドープTa2O5粉末を5mgと、ルテニウムを核とする錯体触媒[Ru(bpy)2(CO)2]2+(bpy=2,2’−bipyridine)を濃度0.05mM相当入れた後に、CO2ガスを溶液中に15分間通気し溶液中に飽和させ、ゴム栓で密閉した。
8mLサイズの試験管に、アセトニトリルとトリエタノールアミン(TEOA)を5:1の体積比で混合した溶液を4mL入れ、さらに実施例1で使用したものと同じニッケル含有酸化亜鉛の粉末を5mgと、ルテニウムを核とし、ビピリジン配位子を有する錯体[Ru(bpy)2(CO)2]2+(bpy=2,2’−bipyridine)を濃度0.05mM相当入れた後に、CO2ガスを溶液中に15分間通気し溶液中に飽和させ、ゴム栓で密閉した。
実施例6からトリエタノールアミン(TEOA)を除いた状態をゴム栓で密閉した。
<比較例6>
実施例6からCO2ガスの代わりにアルゴンガス(Ar)を溶液中に15分間通気し溶液中に飽和させ、ゴム栓で密閉した。
<比較例7>
実施例6から錯体[Ru(bpy)2(CO)2]2+を除いた状態をゴム栓で密閉した。
<比較例8>
比較例7にさらに、CO2ガスの代わりにアルゴンガス(Ar)を溶液中に15分間通気し溶液中に飽和させ、ゴム栓で密閉した。
<比較例9>
実施例7から、CO2ガスの代わりにアルゴンガス(Ar)を溶液中に15分間通気し溶液中に飽和させ、ゴム栓で密閉した。
<比較例10>
実施例6から、NドープTa2O5粉末を除いた状態をゴム栓で密閉した。
<比較例11>
比較例10にさらに、CO2ガスの代わりにアルゴンガス(Ar)を溶液中に15分間通気し溶液中に飽和させ、ゴム栓で密閉した。
<比較例12>
実施例6から、NドープTa2O5粉末と錯体触媒[Ru(bpy)2(CO)2]2+を除いた状態をゴム栓で密閉した。
<比較例13>
比較例12にさらに、CO2ガスの代わりにアルゴンガス(Ar)を溶液中に15分間通気し溶液中に飽和させ、ゴム栓で密閉した。
Claims (9)
- 半導体と、基材と、を、互いに電子をやりとりできる状態で共存させ、少なくとも前記半導体に光を照射することによって前記半導体に生じた励起電子が前記基材に移動することにより前記基材が触媒反応を呈する光触媒体。
- 請求項1に記載の光触媒体であって、前記半導体と前記基材とが接触することを特徴とする光触媒体。
- 請求項1に記載の光触媒体であって、前記半導体と前記基材とが接合されていることを特徴とする光触媒体。
- 請求項1〜3のいずれか1つに記載の光触媒体であって、
前記半導体の伝導帯の最下端のエネルギー準位値から前記電子によって占有されていない分子軌道のうち最もエネルギーの低い準位値を引いた値が0.2電子ボルト以下であることを特徴とする光触媒体。 - 請求項1〜4のいずれか1つに記載の光触媒体であって、
前記基材は、金属錯体であることを特徴とする光触媒体。 - 請求項1〜5のいずれか1つに記載の光触媒体であって、
前記基材は、レニウム錯体又はルテニウム錯体であることを特徴とする光触媒体。 - 請求項1〜6のいずれか1つに記載の光触媒体であって、
前記半導体は、ニッケル含有硫化亜鉛、銅含有硫化亜鉛、窒化タンタル、酸窒化タンタル、酸化タンタル、硫化亜鉛、リン化ガリウム、リン化インジウム、炭化ケイ素、酸化鉄、銅の酸化物の少なくとも1つを含むことを特徴とする光触媒体。 - 請求項1〜6のいずれか1つに記載の光触媒体であって、
前記基材側における触媒反応は還元反応であることを特徴とする光触媒体。 - 半導体と、基材と、が接合された構造を有し、
前記半導体に光を照射することによって生じた励起電子が前記基材に移動することにより炭素含有化合物を還元する光触媒体。
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US8652989B2 (en) | 2014-02-18 |
US20110143929A1 (en) | 2011-06-16 |
CN102119055B (zh) | 2015-04-22 |
WO2010018871A1 (en) | 2010-02-18 |
CN102119055A (zh) | 2011-07-06 |
JP5493572B2 (ja) | 2014-05-14 |
EP2310125A1 (en) | 2011-04-20 |
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