JP5490042B2 - 水分解用光触媒及びそれを含む水分解用光電極 - Google Patents
水分解用光触媒及びそれを含む水分解用光電極 Download PDFInfo
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims description 100
- 239000011941 photocatalyst Substances 0.000 title claims description 81
- 150000003346 selenoethers Chemical class 0.000 claims description 50
- 229910052733 gallium Inorganic materials 0.000 claims description 17
- 239000000758 substrate Substances 0.000 claims description 15
- 229910005543 GaSe Inorganic materials 0.000 claims description 9
- 229910052697 platinum Inorganic materials 0.000 claims description 9
- 229910052703 rhodium Inorganic materials 0.000 claims description 8
- 108010052418 (N-(2-((4-((2-((4-(9-acridinylamino)phenyl)amino)-2-oxoethyl)amino)-4-oxobutyl)amino)-1-(1H-imidazol-4-ylmethyl)-1-oxoethyl)-6-(((-2-aminoethyl)amino)methyl)-2-pyridinecarboxamidato) iron(1+) Proteins 0.000 claims description 4
- 238000000354 decomposition reaction Methods 0.000 claims description 4
- 230000003287 optical effect Effects 0.000 claims description 3
- 239000003054 catalyst Substances 0.000 claims description 2
- 239000010410 layer Substances 0.000 description 44
- 239000011669 selenium Substances 0.000 description 42
- 239000000463 material Substances 0.000 description 27
- 229910052739 hydrogen Inorganic materials 0.000 description 24
- 239000001257 hydrogen Substances 0.000 description 23
- 238000005259 measurement Methods 0.000 description 23
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 22
- 229910052751 metal Inorganic materials 0.000 description 19
- 239000002184 metal Substances 0.000 description 16
- 238000006243 chemical reaction Methods 0.000 description 15
- 229910052711 selenium Inorganic materials 0.000 description 14
- 238000010521 absorption reaction Methods 0.000 description 13
- 239000004065 semiconductor Substances 0.000 description 13
- 238000000151 deposition Methods 0.000 description 12
- 238000010586 diagram Methods 0.000 description 12
- 230000000694 effects Effects 0.000 description 12
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Substances [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 11
- 239000010409 thin film Substances 0.000 description 10
- DVRDHUBQLOKMHZ-UHFFFAOYSA-N chalcopyrite Chemical compound [S-2].[S-2].[Fe+2].[Cu+2] DVRDHUBQLOKMHZ-UHFFFAOYSA-N 0.000 description 9
- 229910052951 chalcopyrite Inorganic materials 0.000 description 9
- 229910052738 indium Inorganic materials 0.000 description 9
- 238000000034 method Methods 0.000 description 9
- 238000006722 reduction reaction Methods 0.000 description 9
- 229910052717 sulfur Inorganic materials 0.000 description 9
- 230000008021 deposition Effects 0.000 description 8
- 229910052709 silver Inorganic materials 0.000 description 8
- 239000010936 titanium Substances 0.000 description 8
- 150000001875 compounds Chemical class 0.000 description 7
- 238000004519 manufacturing process Methods 0.000 description 7
- 238000007254 oxidation reaction Methods 0.000 description 7
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 6
- 239000013078 crystal Substances 0.000 description 6
- 230000003647 oxidation Effects 0.000 description 6
- 230000009467 reduction Effects 0.000 description 6
- 239000000203 mixture Substances 0.000 description 5
- 238000001451 molecular beam epitaxy Methods 0.000 description 5
- 230000001699 photocatalysis Effects 0.000 description 5
- 239000005361 soda-lime glass Substances 0.000 description 5
- 229910021607 Silver chloride Inorganic materials 0.000 description 4
- 239000007789 gas Substances 0.000 description 4
- 230000001678 irradiating effect Effects 0.000 description 4
- 238000001420 photoelectron spectroscopy Methods 0.000 description 4
- 238000006479 redox reaction Methods 0.000 description 4
- HKZLPVFGJNLROG-UHFFFAOYSA-M silver monochloride Chemical compound [Cl-].[Ag+] HKZLPVFGJNLROG-UHFFFAOYSA-M 0.000 description 4
- BUGBHKTXTAQXES-UHFFFAOYSA-N Selenium Chemical compound [Se] BUGBHKTXTAQXES-UHFFFAOYSA-N 0.000 description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 238000002441 X-ray diffraction Methods 0.000 description 3
- 239000007864 aqueous solution Substances 0.000 description 3
- 239000001569 carbon dioxide Substances 0.000 description 3
- 229910002092 carbon dioxide Inorganic materials 0.000 description 3
- 239000008151 electrolyte solution Substances 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 3
- 150000002500 ions Chemical class 0.000 description 3
- 150000002739 metals Chemical class 0.000 description 3
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- 239000000843 powder Substances 0.000 description 3
- 238000004544 sputter deposition Methods 0.000 description 3
- 229910052719 titanium Inorganic materials 0.000 description 3
- 229940126062 Compound A Drugs 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- NLDMNSXOCDLTTB-UHFFFAOYSA-N Heterophylliin A Natural products O1C2COC(=O)C3=CC(O)=C(O)C(O)=C3C3=C(O)C(O)=C(O)C=C3C(=O)OC2C(OC(=O)C=2C=C(O)C(O)=C(O)C=2)C(O)C1OC(=O)C1=CC(O)=C(O)C(O)=C1 NLDMNSXOCDLTTB-UHFFFAOYSA-N 0.000 description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 2
- 239000012790 adhesive layer Substances 0.000 description 2
- 230000008859 change Effects 0.000 description 2
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- 239000002803 fossil fuel Substances 0.000 description 2
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- 230000031700 light absorption Effects 0.000 description 2
- 229910001092 metal group alloy Inorganic materials 0.000 description 2
- 229910021645 metal ion Inorganic materials 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
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- 238000001055 reflectance spectroscopy Methods 0.000 description 2
- 230000002441 reversible effect Effects 0.000 description 2
- 239000004332 silver Substances 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 238000001771 vacuum deposition Methods 0.000 description 2
- -1 GaSe or Ga 2 Se 3 Chemical class 0.000 description 1
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 description 1
- 241000511976 Hoya Species 0.000 description 1
- 229910052774 Proactinium Inorganic materials 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 229910052787 antimony Inorganic materials 0.000 description 1
- 125000004429 atom Chemical group 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000000903 blocking effect Effects 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- 229910052794 bromium Inorganic materials 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- 229910052792 caesium Inorganic materials 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 150000001768 cations Chemical class 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- ZZEMEJKDTZOXOI-UHFFFAOYSA-N digallium;selenium(2-) Chemical compound [Ga+3].[Ga+3].[Se-2].[Se-2].[Se-2] ZZEMEJKDTZOXOI-UHFFFAOYSA-N 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 239000003822 epoxy resin Substances 0.000 description 1
- 230000005284 excitation Effects 0.000 description 1
- 239000010408 film Substances 0.000 description 1
- 229910052731 fluorine Inorganic materials 0.000 description 1
- 238000004817 gas chromatography Methods 0.000 description 1
- 229910052732 germanium Inorganic materials 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 229910052735 hafnium Inorganic materials 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- GPRLSGONYQIRFK-UHFFFAOYSA-N hydron Chemical compound [H+] GPRLSGONYQIRFK-UHFFFAOYSA-N 0.000 description 1
- 229910052740 iodine Inorganic materials 0.000 description 1
- WABPQHHGFIMREM-UHFFFAOYSA-N lead(0) Chemical compound [Pb] WABPQHHGFIMREM-UHFFFAOYSA-N 0.000 description 1
- 229910052744 lithium Inorganic materials 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 238000001755 magnetron sputter deposition Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- AHKZTVQIVOEVFO-UHFFFAOYSA-N oxide(2-) Chemical compound [O-2] AHKZTVQIVOEVFO-UHFFFAOYSA-N 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 238000002256 photodeposition Methods 0.000 description 1
- 229920000647 polyepoxide Polymers 0.000 description 1
- 229910052700 potassium Inorganic materials 0.000 description 1
- 229910052761 rare earth metal Inorganic materials 0.000 description 1
- 230000004044 response Effects 0.000 description 1
- 229910052701 rubidium Inorganic materials 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 229910052712 strontium Inorganic materials 0.000 description 1
- 239000000725 suspension Substances 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- 229910052714 tellurium Inorganic materials 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 238000002371 ultraviolet--visible spectrum Methods 0.000 description 1
- 238000007738 vacuum evaporation Methods 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- 238000007740 vapor deposition Methods 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
- 229910052724 xenon Inorganic materials 0.000 description 1
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
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Description
(1)Gaセレン化物、Ag−Gaセレン化物、又はそれらの両方を含有し、前記Gaセレン化物がGaSe、Ga 2 Se 3 、及びそれらの組み合わせからなる群より選択される、水分解用光触媒。
(2)Gaセレン化物とAg−Gaセレン化物の両方を含有する、上記(1)に記載の水分解用光触媒。
(3)前記Gaセレン化物がGaSeである、上記(1)又は(2)に記載の水分解用光触媒。
(4)前記Ag−Gaセレン化物がAgGaSe2、AgGa5Se8、及びそれらの組み合わせからなる群より選択される、上記(1)〜(3)のいずれか1つに記載の水分解用光触媒。
(5)前記Ag−Gaセレン化物がAgGaSe2である、上記(4)に記載の水分解用光触媒。
(6)前記Gaセレン化物がGa 2 Se 3 であり、前記Ag−Gaセレン化物がAgGa 5 Se 8 である、上記(1)又は(2)に記載の水分解用光触媒。
(7)Rh及びPtの少なくとも1種が担持された、上記(1)〜(6)のいずれか1つに記載の水分解用光触媒。
(8)基板と、該基板上に形成された導電層と、該導電層上に形成され、上記(1)〜(7)のいずれか1つに記載の水分解用光触媒からなる光触媒層とを含む、水分解用光電極。
還元反応 H+ + e- → 1/2H2 E0=0V
酸化反応 H2O → 1/2O2 + 2H+ + 2e- E0=1.23V
[光電極の作製]
まず、エタノール中で超音波洗浄した面積5×10mm2のソーダライムガラス(SLG)を基板として使用し、これをRF−マグネトロンスパッタ装置のチャンバー内に挿入して、当該チャンバー内を10-4Pa台の圧力まで真空引きした。次いで、基板温度200℃、スパッタパワー100W、Ar分圧8×10-2Paの条件下において、ArプラズマによりSLG基板上にTiを5分間スパッタして接着層としてのTi層を堆積させ、続いて当該Ti層上にMoを20分間スパッタして集電極としてのMo層を堆積させた。
実施例2〜8では、Mo/Ti/SLG基板上へのGaの真空蒸着前に、Agを0.4〜0.5nm/sの堆積速度でMo層上に真空蒸着し、Ag/Ga比(原子比)=0.06〜1.20となるような厚さおいてAg薄膜とGa薄膜を堆積させたこと以外は実施例1と同様にして、Ag/Ga比がそれぞれ0.06、0.17、0.24、0.55、0.60、0.77及び1.20の光触媒層を備えた水分解用光電極を得た。
実施例1〜8において得られた各試料について、X線回折(XRD)によってそれらの測定を行った。図4は、実施例1〜8の各試料に関するXRDパターンを示す図である。
本実施例では、実施例1〜8と同様にして光触媒層に含まれるAgとGaの原子比(Ag/Ga比)が(a)0、(b)0.11、(c)0.17、(d)0.19、(e)0.23、(f)0.48、(g)0.59、(h)0.65及び(i)0.75である合計9つの試料を作製し、それらの各試料について伝導帯下端(CBM)と価電子帯上端(VBM)を算出した。
[光電気化学測定]
本実施例では、Ag/Ga比=0.15の光触媒層を備えた水分解用光電極を実施例1〜8と同様にして作製し、図9に示す装置を用いて光電気化学測定を行った。なお、当該光電気化学測定に際し、上記の水分解用光電極のMo層にInを用いて導線を接着し、不要部分をエポキシ樹脂で被覆して電解液と接触しないようにした。
次に、上記の光電気化学測定において最も高い水分解活性を示したRh担持光電極について、Ag/Ga比を変化させた場合の影響について調べた。具体的には、Ag/Ga比がそれぞれ0、0.06、0.15及び0.55である光触媒層に上で説明したのと同様にしてRhを担持した水分解用光電極を作製し、それらの各水分解用光電極に関して光電気化学測定を行った。その結果を図11に示す。また、図11から得られた各水分解用光電極の光電流開始電位(VRHE)(図11において矢印で示す)の値を下表2にまとめる。
次に、Ag/Ga比=0.15のRh担持光電極を用いた光電気化学測定において生成したガスを分析した結果を図12に示す。
2 Ga
3 Se
Claims (8)
- Gaセレン化物、Ag−Gaセレン化物、又はそれらの両方を含有し、前記Gaセレン化物がGaSe、Ga 2 Se 3 、及びそれらの組み合わせからなる群より選択される、水分解用光触媒。
- Gaセレン化物とAg−Gaセレン化物の両方を含有する、請求項1に記載の水分解用光触媒。
- 前記Gaセレン化物がGaSeである、請求項1又は2に記載の水分解用光触媒。
- 前記Ag−Gaセレン化物がAgGaSe2、AgGa5Se8、及びそれらの組み合わせからなる群より選択される、請求項1〜3のいずれか1項に記載の水分解用光触媒。
- 前記Ag−Gaセレン化物がAgGaSe2である、請求項4に記載の水分解用光触媒。
- 前記Gaセレン化物がGa 2 Se 3 であり、前記Ag−Gaセレン化物がAgGa 5 Se 8 である、請求項1又は2に記載の水分解用光触媒。
- Rh及びPtの少なくとも1種が担持された、請求項1〜6のいずれか1項に記載の水分解用光触媒。
- 基板と、該基板上に形成された導電層と、該導電層上に形成され、請求項1〜7のいずれか1項に記載の水分解用光触媒からなる光触媒層とを含む、水分解用光電極。
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JP2011052967A JP5490042B2 (ja) | 2011-03-10 | 2011-03-10 | 水分解用光触媒及びそれを含む水分解用光電極 |
PCT/JP2012/054685 WO2012121034A1 (en) | 2011-03-10 | 2012-02-20 | Photocatalyst for water splitting comprising gallium selenide and photoelectrode for water splitting comprising the same |
CN201280012655.XA CN103415339B (zh) | 2011-03-10 | 2012-02-20 | 包含镓的硒化物的水分解用光催化剂和包含所述光催化剂的水分解用光电极 |
DE112012001177.5T DE112012001177T5 (de) | 2011-03-10 | 2012-02-20 | Fotokatalysator zum Spalten von Wasser enthaltend Galliumselenid und Fotoelektrode zum Spalten von Wasser enthaltend denselben |
US14/004,252 US20140001036A1 (en) | 2011-03-10 | 2012-02-20 | Photocatalyst for water splitting comprising gallium selenide and photoelectrode for water splitting comprising the same |
US14/640,628 US9975115B2 (en) | 2011-03-10 | 2015-03-06 | Photocatalyst for water splitting comprising gallium selenide and photoelectrode for water splitting comprising the same |
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