[1]陈雪皎,彭伟,陆君涛,等.半夹心钌分子催化剂的水氧化电催化[J].华侨大学学报(自然科学版),2020,41(6):779-783.[doi:10.11830/ISSN.1000-5013.202009025]
 CHEN Xuejiao,PENG Wei,LU Juntao,et al.Half-Sandwich Ruthenium Molecular Catalyst Towards Water Oxidation Electrolysis[J].Journal of Huaqiao University(Natural Science),2020,41(6):779-783.[doi:10.11830/ISSN.1000-5013.202009025]
点击复制

半夹心钌分子催化剂的水氧化电催化()
分享到:

《华侨大学学报(自然科学版)》[ISSN:1000-5013/CN:35-1079/N]

卷:
第41卷
期数:
2020年第6期
页码:
779-783
栏目:
出版日期:
2020-11-20

文章信息/Info

Title:
Half-Sandwich Ruthenium Molecular Catalyst Towards Water Oxidation Electrolysis
文章编号:
1000-5013(2020)06-0779-05
作者:
陈雪皎1 彭伟2 陆君涛2 庄林2
1. 华侨大学 材料科学与工程学院, 福建 厦门 361021;2. 武汉大学 化学与分子科学学院, 湖北 武汉 430072
Author(s):
CHEN Xuejiao1 PENG Wei2 LU Juntao2 ZHUANG Lin2
1. College of Materials Science and Engineering, Huaqiao University, Xiamen 361021, China; 2. College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, China
关键词:
分子催化剂 半夹心钌配合物 微分电化学质谱 水氧化反应 电催化
Keywords:
molecular catalyst half-sandwich ruthenium complex differential electrochemical mass spectrometry water oxidation reaction electrocatalysis
分类号:
O646.5
DOI:
10.11830/ISSN.1000-5013.202009025
文献标志码:
A
摘要:
设计和合成以五甲基环戊二烯基(Cp*)半夹心钌配合物为代表的一种具有开放的空间结构和高电荷密度的分子催化剂,通过对配体的调控,成功筛选出具有良好水氧化电催化活性、易固载到电极表面且在强碱性环境下抗水解的[Cp*Ru(PPh3)2Cl]Cl配合物分子.电化学和在线微分电化学质谱实验表明:该分子可提供易于被进攻Ru(Ⅴ)活性中心,显著加速水氧化生成O2的反应速率.
Abstract:
A half-sandwich ruthenium complex for the water oxidation reaction electrolysis with one pentamethylcyclopentadienyl(Cp*)ligand was designed and prepared, which is featured with an open geometric configuration and a high density of charge. By tuning the other ligands, a [Cp*Ru(PPh3)2Cl]Cl molecule was screened successfully which encompassed a superior catalytic activity, a facile fixation to the electrode, and a high resistance to the hydrolysis reaction under the strong-alkaline condition. Combining the electrochemical and on-line differential electrochemical mass spectrometry studies, it is proposed that this molecular Ru catalyst can provide accessible Ru(Ⅴ)active center which can remarkably accelerate the water oxidation to O2.

参考文献/References:

[1] DUAN Lele,BOZOGLIAN F,MANDAL S,et al.A molecular ruthenium catalyst with water-oxidation activity comparable to that of photosystem Ⅱ[J].Nature Chemistry,2012,4(5):418-423.DOI:10.1038/nchem.1301.
[2] BARBER J,TRAN P D.From natural to artificial photosynthesis[J].Journal of the Royal Society Interface,2013,10(81):1-15.
[3] BONKE S A,WIECHEN M,MACFARLANE D R,et al.Renewable fuels from concentrated solar power: Towards practical artificial photosynthesis[J].Energy and Environmental Science,2015,8(9):2791-2796.DOI:10.1039/C5 EE02214B.
[4] KANAN M W,NOCERA D G.In situ formation of an oxygen-evolving catalyst in neutral water containing phosphate and Co2+[J].Science,2008,321:1072-1075.DOI:10.1126/science.1162018.
[5] DUAN Lele,TONG Lianpeng,XU Yunhua,et al.Visible light-driven water oxidation-from molecular catalysts to photoelectrochemical cells[J].Energy and Environmental Science,2011,4(9):3296-3313.DOI:10.1039/C1EE0127 6b.
[6] DENG Xiaohui,TUYSUZ H.Cobalt-oxide-based materials as water oxidation catalyst: Recent progress and challenges[J].ACS Catalysis,2014,4(10):3701-3714.DOI:10.1021/cs500713d.
[7] SAVEANT J M.Molecular catalysis of electrochemical reactions: Mechanistic aspects[J].Chemical Reviews,2008,108(7):2348-2378.DOI:10.1021/cr068079z.
[8] CHEN Xuejiao,REN Xiaodi,LIU Zilong,et al.Promoting the photoanode efficiency for water splitting by combining hematite and molecular Ru catalysts[J].Electrochemistry Communications,2013,27:148-151.DOI:10.1016/j.elecom.2012.11.026.
[9] THOI V S,SUN Yujie,LONG J R,et al.Complexes of earth-abundant metals for catalytic electrochemical hydrogen generation under aqueous conditions[J].Chemical Society Reviews,2013,42(6):2388-2400.DOI:10.1039/c2cs352 72a.
[10] ZHANG Biaobiao,SUN Licheng.Artificial photosynthesis: Opportunities and challenges of molecular catalysts[J].Chemical Society Reviews,2019,48(7):2216-2264.DOI:10.1039/c8cs00897c.
[11] ARTERO V,FONTECAVE M.Solar fuels generation and molecular systems: Is it homogeneous or heterogeneous catalysis?[J].Chemical Society Reviews,2013,42(6):2338-2356.DOI:10.1039/c2cs35334b.

备注/Memo

备注/Memo:
收稿日期: 2020-09-12
通信作者: 陈雪皎(1984-),女,讲师,博士,主要从事能源化学相关的电催化与谱学电化学的研究.E-mail:xjchen@hqu.edu.cn.
基金项目: 福建省自然科学基金面上资助项目(2019J01058); 华侨大学科技创新能力提升计划项目(ZQN-PY507); 华侨大学高层次人才科研启动费项目(605-50Y17061)
更新日期/Last Update: 2020-11-20