贵金属负载TiO<sub>2</sub>对光催化还原CO<sub>2</sub>选择性的影响

引用本文: 郝瑞鹏, 杨朋举, 王志坚, 朱珍平. 贵金属负载TiO₂对光催化还原CO₂选择性的影响[J]. 燃料化学学报, 2015, 43(1): 94-99. shu

Citation: HAO Rui-peng, YANG Peng-ju, WANG Zhi-jian, ZHU Zhen-ping. Effect of noble metals loaded TiO₂ on the selectivity of photocatalytic CO₂ reduction[J]. Journal of Fuel Chemistry and Technology, 2015, 43(1): 94-99. shu

贵金属负载TiO₂对光催化还原CO₂选择性的影响

郝瑞鹏 ^1,2, ,
杨朋举 ^1,2, ,
王志坚 ^{1,
,} ,
朱珍平 ^{1,
,}

通讯作者: 王志坚,Tel:0351-4045918,Fax:0351-4151663,E-mail:wangzhijian@sxicc.ac.cn;朱珍平,Tel:0351-4048715,Fax:0351-4151663,E-mail:zpzhu@sxicc.ac.cn.; 王志坚,Tel:0351-4045918,Fax:0351-4151663,E-mail:wangzhijian@sxicc.ac.cn;朱珍平,Tel:0351-4048715,Fax:0351-4151663,E-mail:zpzhu@sxicc.ac.cn.

基金项目:
国家自然科学基金(21173250). (21173250)

摘要: 利用光沉积方法在TiO₂表面分别负载1%(质量分数) Pt、Pd、Au和Ag助催化剂.用TEM、XRD、UV-vis等技术对催化剂进行了表征,并利用连续瞬态电流时间响应和线性扫描伏安法等电化学方法,对贵金属负载的TiO₂光催化剂在光照条件下的电流响应强度及电催化析氢电位等特性加以测试.分析了贵金属助催化剂对光催化还原CO₂性能的差异.结果表明,负载贵金属助催化剂能显著加速光生电子空穴的分离,降低复合率;另外,助催化剂对还原CO₂选择性的顺序为Ag>Au>Pd>Pt.贵金属助催化剂还原CO₂的加氢选择性和析氢过电位存在相关性,即越不利于析氢过程的助催化剂,其催化CO₂加氢还原产物的选择性越高.

关键词:

助催化剂
/ TiO₂
/ 光催化
/ 还原CO₂

English

Effect of noble metals loaded TiO₂ on the selectivity of photocatalytic CO₂ reduction

1.
1. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China;

Corresponding author: 王志坚,Tel:0351-4045918,Fax:0351-4151663,E-mail:wangzhijian@sxicc.ac.cn;朱珍平,Tel:0351-4048715,Fax:0351-4151663,E-mail:zpzhu@sxicc.ac.cn.; 王志坚,Tel:0351-4045918,Fax:0351-4151663,E-mail:wangzhijian@sxicc.ac.cn;朱珍平,Tel:0351-4048715,Fax:0351-4151663,E-mail:zpzhu@sxicc.ac.cn.

Received Date: 25 September 2014
Fund Project:
国家自然科学基金(21173250).

Abstract: The TiO₂ photocatalyst loaded with 1% Pt, Pd, Au, Ag have been prepared by photo deposition method. The catalysts are characterized with X-ray diffraction (XRD), transmission electron microscopy (TEM), and UV-vis spectrometer. The electro-catalytic performance for hydrogen production and photo electrochemical performance are investigated by using linear sweep voltammetry method and continuous transient current-time response method. The performance of photocatalytic CO₂ reduction on TiO₂ loaded with different noble metals are discussed. The results show that loading noble metal on TiO₂ can significantly accelerate the separation of photo production electron and hole and reduce the recombination rate. Furthermore, the sequence of cocatalysts selective reduction for CO₂ is Ag>Au>Pd>Pt. A negative correlation between the selectivity of CO₂ hydrogenation and hydrogen production has been discovered. The cocatalyst which has advantage to hydrogen evolution process goes against the selectivity of CO₂ hydrogenation.

Key words:

1. [1] FUJISHIMA A, HONDA K. Electrochemical photolysis of water at a semiconductor electrode[J]. Nature, 1972, 238(5358): 37-38.[1] FUJISHIMA A, HONDA K. Electrochemical photolysis of water at a semiconductor electrode[J]. Nature, 1972, 238(5358): 37-38.
2. [2] INOUE T, FUJISHIMA A, KONISHI S, HONDA K. Photoelectrocatalytic reduction of carbon dioxide in aqueous suspensions of semiconductor powders[J]. Nature, 1979, 277(5698): 637-638.[2] INOUE T, FUJISHIMA A, KONISHI S, HONDA K. Photoelectrocatalytic reduction of carbon dioxide in aqueous suspensions of semiconductor powders[J]. Nature, 1979, 277(5698): 637-638.
3. [3] NAVALÓN S, DHAKSHINAMOORTHY A, ÁLVARO M, GARCIA H. Photocatalytic CO₂ reduction using non-titanium metal oxides and sulfides[J]. ChemSusChem, 2013, 6(4): 562-577.[3] NAVALÓN S, DHAKSHINAMOORTHY A, ÁLVARO M, GARCIA H. Photocatalytic CO₂ reduction using non-titanium metal oxides and sulfides[J]. ChemSusChem, 2013, 6(4): 562-577.
4. [4] HABISREUTINGER S N, SCHMIDT-MENDE L, STOLARCZYK J K. Photocatalytic reduction of CO₂ on TiO₂ and other semiconductors[J]. Angew Chem Int Ed, 2013, 52(29): 7372-7408.[4] HABISREUTINGER S N, SCHMIDT-MENDE L, STOLARCZYK J K. Photocatalytic reduction of CO₂ on TiO₂ and other semiconductors[J]. Angew Chem Int Ed, 2013, 52(29): 7372-7408.
5. [5] ZHAI Q G, XIE S J, FAN W Q, ZHANG Q H, WANG Y, DENG W P, WANG Y. Photocatalytic conversion of carbon dioxide with water into methane: Platinum and copper(i) oxide co-catalysts with a core-shell structure[J]. Angew Chem Int Ed, 2013, 52(22): 5776-5779.[5] ZHAI Q G, XIE S J, FAN W Q, ZHANG Q H, WANG Y, DENG W P, WANG Y. Photocatalytic conversion of carbon dioxide with water into methane: Platinum and copper(i) oxide co-catalysts with a core-shell structure[J]. Angew Chem Int Ed, 2013, 52(22): 5776-5779.
6. [6] TU W G, ZHOU Y, ZOU Z G. Photoconversion: Photocatalytic conversion of CO₂ into renewable hydrocarbon fuels: State-of-the-art accomplishment, challenges, and prospects[J]. Adv Mat, 2014, 26(27): 4598-4598.[6] TU W G, ZHOU Y, ZOU Z G. Photoconversion: Photocatalytic conversion of CO₂ into renewable hydrocarbon fuels: State-of-the-art accomplishment, challenges, and prospects[J]. Adv Mat, 2014, 26(27): 4598-4598.
7. [7] IIZUKA K, WATO T, MISEKI Y, SAITO K, KUDO A. Photocatalytic reduction of carbon dioxide over Ag cocatalyst-loaded ALa₄Ti₄O₁₅(A=Ca, Sr, and Ba) using water as a reducing reagent[J]. J Am Chem Soc, 2011, 133(51): 20863-20868.[7] IIZUKA K, WATO T, MISEKI Y, SAITO K, KUDO A. Photocatalytic reduction of carbon dioxide over Ag cocatalyst-loaded ALa₄Ti₄O₁₅(A=Ca, Sr, and Ba) using water as a reducing reagent[J]. J Am Chem Soc, 2011, 133(51): 20863-20868.
8. [8] ZHOU H, GUO J J, LI P, FAN T X, ZHANG D, YE J H. Leaf-architectured 3D hierarchical artificial photosynthetic system of perovskite titanates towards CO₂ photoreduction into hydrocarbon fuels[J]. Sci Rep, 2013, 3: 1667.[8] ZHOU H, GUO J J, LI P, FAN T X, ZHANG D, YE J H. Leaf-architectured 3D hierarchical artificial photosynthetic system of perovskite titanates towards CO₂ photoreduction into hydrocarbon fuels[J]. Sci Rep, 2013, 3: 1667.
9. [9] HE J H, ICHINOSE I, KUNITAKE T, NAKAO A. In situ synthesis of noble metal nanoparticles in ultrathin TiO₂-Gel films by a combination of ion-exchange and reduction processes[J]. Langmuir, 2002, 18(25): 10005-10010.[9] HE J H, ICHINOSE I, KUNITAKE T, NAKAO A. In situ synthesis of noble metal nanoparticles in ultrathin TiO₂-Gel films by a combination of ion-exchange and reduction processes[J]. Langmuir, 2002, 18(25): 10005-10010.
10. [10] LIU Z W, HOU W B, PAVASKAR P, AYKOL M, CRONIN S B. Plasmon resonant enhancement of photocatalytic water splitting under visible illumination[J]. Nano Lett, 2011, 11(3): 1111-1116.[10] LIU Z W, HOU W B, PAVASKAR P, AYKOL M, CRONIN S B. Plasmon resonant enhancement of photocatalytic water splitting under visible illumination[J]. Nano Lett, 2011, 11(3): 1111-1116.
11. [11] YUI T, KAN A, SAITOH C, KOIKE K, IBUSUKI T, ISHITANI O. Photochemical reduction of CO₂ Using TiO₂: Effects of organic adsorbates on TiO₂ and deposition of Pd onto TiO₂[J]. Acs Appl Mat Int, 2011, 3(7): 2594-2600.[11] YUI T, KAN A, SAITOH C, KOIKE K, IBUSUKI T, ISHITANI O. Photochemical reduction of CO₂ Using TiO₂: Effects of organic adsorbates on TiO₂ and deposition of Pd onto TiO₂[J]. Acs Appl Mat Int, 2011, 3(7): 2594-2600.
12. [12] INDRAKANTI V P, KUBICKI J D, SCHOBERT H H. Photoinduced activation of CO₂ on Ti-based heterogeneous catalysts: Current state, chemical physics-based insights and outlook[J]. Energy Environ Sci, 2009, 2(7): 745-758.[12] INDRAKANTI V P, KUBICKI J D, SCHOBERT H H. Photoinduced activation of CO₂ on Ti-based heterogeneous catalysts: Current state, chemical physics-based insights and outlook[J]. Energy Environ Sci, 2009, 2(7): 745-758.
13. [13] IKEDA S, TAKAGI T, ITO K. Selective formation of formic-acid, oxalic-acid, and carbon-monoxide by electrochemical reduction of carbon-dioxide[J]. Bull Chem Soc Jpn, 1987, 60(7): 2517-2522.[13] IKEDA S, TAKAGI T, ITO K. Selective formation of formic-acid, oxalic-acid, and carbon-monoxide by electrochemical reduction of carbon-dioxide[J]. Bull Chem Soc Jpn, 1987, 60(7): 2517-2522.
14. [14] YANG J H, WANG D G, HAN H X, LI C.Roles of cocatalysts in photocatalysis and photoelectrocatalysis[J]. Acc Chem Res, 2013, 46(8): 1900-1909.[14] YANG J H, WANG D G, HAN H X, LI C.Roles of cocatalysts in photocatalysis and photoelectrocatalysis[J]. Acc Chem Res, 2013, 46(8): 1900-1909.
15. [15] PETERSON A A, NORSKOV J K. Activity descriptors for CO₂ electroreduction to methane on transition-metal catalysts[J]. J Phys Chem Lett, 2012, 3(2): 251-258.[15] PETERSON A A, NORSKOV J K. Activity descriptors for CO₂ electroreduction to methane on transition-metal catalysts[J]. J Phys Chem Lett, 2012, 3(2): 251-258.
16. [16] HORI Y, WAKEBE H, TSUKAMOTO T, KOGA O. Electrocatalytic process of CO selectivity in electrochemical reduction of CO₂ at metal-electrodes in aqueous-media[J]. Electrochim Acta, 1994, 39(11/12): 1833-1839.[16] HORI Y, WAKEBE H, TSUKAMOTO T, KOGA O. Electrocatalytic process of CO selectivity in electrochemical reduction of CO₂ at metal-electrodes in aqueous-media[J]. Electrochim Acta, 1994, 39(11/12): 1833-1839.
17. [17] WANG W N, AN W J, RAMALINGAM B, MUKHERJEE S, NIEDZWIEDZKI D M, GANGOPADHYAY S, BISWAS P. Size and structure matter: Enhanced CO₂ photoreduction efficiency by size-resolved ultrafine Pt nanoparticles on TiO₂ single crystals[J]. J Am Chem Soc, 2012, 134(27): 11276-11281.[17] WANG W N, AN W J, RAMALINGAM B, MUKHERJEE S, NIEDZWIEDZKI D M, GANGOPADHYAY S, BISWAS P. Size and structure matter: Enhanced CO₂ photoreduction efficiency by size-resolved ultrafine Pt nanoparticles on TiO₂ single crystals[J]. J Am Chem Soc, 2012, 134(27): 11276-11281.

扫一扫看文章

计量

PDF下载量: 0
文章访问数: 0
HTML全文浏览量: 0

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

贵金属负载TiO₂对光催化还原CO₂选择性的影响

English

Effect of noble metals loaded TiO₂ on the selectivity of photocatalytic CO₂ reduction

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

贵金属负载TiO2对光催化还原CO2选择性的影响

English

Effect of noble metals loaded TiO2 on the selectivity of photocatalytic CO2 reduction

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

贵金属负载TiO₂对光催化还原CO₂选择性的影响

Effect of noble metals loaded TiO₂ on the selectivity of photocatalytic CO₂ reduction

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs