Photoelectrochemical reduction of Carbon dioxide by metal-complexes-membrane electrodes

金属配合物膜电极光电化学还原二氧化碳

• 批准号: 06453114
• 负责人: MIZUNO Takayuki
• 金额: $ 4.8万
• 依托单位: MIE UNIVERSITY
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for General Scientific Research (B)
• 财政年份: 1994
• 资助国家: 日本
• 起止时间: 1994 至 1995
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-06453114/
• 关键词: Carbon dioxide; Photocatalytic reduction; Modified membrane electrode; 光光学還元

Object : Phtochemical reduction of CO_2 is considered to be one of the most pro-mising approaches to photochemical conversion and storage of solar energy. An aqucous system of Ruthenium (II) -bipyridine complexes-methylviologen (MV^<2+>) -triethanolamine is one of homogeneous photosinsitized reductions of CO_2. In thissystem tricthanolamine is exhausted as sacrificial electron donor. With a view to search a cyclic system, we study on photoelectrochemical CO_2 reduction using coated membrane electrodes containing complexes and MV^<2+> without sacrificial clectron donor. Additionally photocatalytic reduction of CO_2 was studied using TiO_2 in suspension in liquid CO_2 and supercritical CO_2.Results :1.The electrode covered by the membranes containing Ru (bpy)_3^<2+> and MV^<2+> formed the largest photocurrent in the potential below -0.2 V.This indicates that Ru (bpy)_3^<2+> and MV^<2+> system in the membrane was most effective in generating photoc-urrent.2.In the Ru (bpy)_3^<2+> and MV^<2+> membrane system, exclusively II_2 was found as the reduction product. The electrode electrodeposited Pt or Ru reduced photoelectro-chemically CO_2 to produce malonic acid, acetic acid and formic acid as reduction products.3.We found that CO_2 was reduced by two stage reactions, that is, CO_2 fluid was photoc-atalytically reduced with TiO_2 in suspension and then protonated to formic acid by water addition.

对象：光化学还原CO_2被认为是光化学转化和储存太阳能的最有前途的途径之一。钌（Ⅱ）-联吡啶配合物-甲基紫精（MV^<2+>）-三乙醇胺水体系是一种均匀的CO_2光催化还原体系。在该体系中，三乙醇胺作为牺牲电子给体被耗尽。为了寻找一种循环体系，我们在不牺牲电子给体的情况下，研究了含络合物和MV^<2+>的涂膜电极对CO_2的光电化学还原。结果表明：1. Ru（bpy）_3^<2+>和MV^<2+>膜覆盖的电极在-0.2V以下产生最大光电流，表明膜中Ru（bpy）_3 ^<2 +>和MV ^<2 +>体系产生光电流最有效。电沉积Pt或Ru的电极光电化学还原CO_2，生成丙二酸、乙酸和甲酸作为还原产物。3.我们发现CO_2的还原分为两阶段反应，即CO_2流体在悬浮液中被TiO_2光催化还原，然后通过加水质子化为甲酸。

项目成果

K.Adachi,K.Ohta.T.Mizuno: "Photocatalytic Reduction of CO_2 to Hydrocarbon using Cu-TiO_2" Solar Energy. 53. 187-190 (1994)

K.Adachi,K.Ohta.T.Mizuno：“利用 Cu-TiO_2 光催化还原 CO_2 为碳氢化合物”太阳能。

T.Mizuno,A.Naito,K.Ohta: "Electrochemical reduction of CO_2 in metanol at -30℃" J.Electroanal.Chem.391. 199-201 (1995)

T.Mizuno，A.Naito，K.Ohta：“-30℃下甲醇中CO_2的电化学还原”J.Electroanal.Chem.391（1995）。

T.Mizuno,K.Ohta,A.Sasaki,A.Kawabe: "Effect of temperature on electrochemical reduction of high-pressure CO_2 with In, Sn, and Pb electrodes" Energy Sources. 17. 503-508 (1995)

T.Mizuno,K.Ohta,A.Sasaki,A.Kawabe：“温度对 In、Sn 和 Pb 电极电化学还原高压 CO_2 的影响”能源。

M.Tanahashi,T.Mizuno K.Ohta,A.Saji: "Photoelectrochemical reduction of CO_2 in water by tris (2,2′bipyridine) Ruthenium (II) and methyl viologen incorporated into coated Nafion membranes" Proc.'95 Asian Conf. on Electrochemistry. May 28-31,1995,Osaka. 174

M.Tanahashi、T.Mizuno K.Ohta、A.Saji：“通过三(2,2联吡啶)钌 (II) 和甲基紫精掺入涂层 Nafion 膜对水中 CO_2 进行光电化学还原”Proc.95 亚洲会议1995 年 5 月 28-31 日，大阪。

T.Mizuno, K.Adachi, K.Ohta: "Effect of CO_2 pressure on photocatalytic reduction of CO_2 using TiO_2 in aqueous solutions" J.Photochem.Photobio.A Chem.(in press).

T.Mizuno、K.Adachi、K.Ohta：“CO_2 压力对水溶液中使用 TiO_2 光催化还原 CO_2 的影响”J.Photochem.Photobio.A Chem.（印刷中）。