中国科学院化学研究所机构知识库
Advanced  
ICCAS OpenIR  > 光化学实验室  > 期刊论文
题名: Enhanced proton and electron reservoir abilities of polyoxometalate grafted on graphene for high-performance hydrogen evolution
作者: Liu, Rongji1; Zhang, Guangjin1; Cao, Hongbin1; Zhang, Suojiang1; Xie, Yongbing1; Haider, Ali2; Kortz, Ulrich2; Chen, Banghao3; Dalal, Naresh S.3; Zhao, Yongsheng4; Zhi, Linjie5; Wu, Cai-Xia6; Yan, Li-Kai6; Su, Zhongmin6; Keita, Bineta7
刊名: ENERGY & ENVIRONMENTAL SCIENCE
发表日期: 2016
卷: 9, 期:3, 页:1012-1023
收录类别: SCI
英文摘要: A beneficial "microenvironment effect" on the efficiency of confined electrocatalysts is predicted by theory. However, examples of its experimental confirmation are scarce for catalysts based on polyoxometalates for the hydrogen evolution reaction (HER). For this purpose, the cyclic 48-tungsto-8-phosphate [H7P8W48O184](33) (P8W48) was fixed in a 3D configuration on reduced graphene oxide sheets (rGO) to boost its HER activity. The HRTEM imaging and the solid state P-31 NMR spectrum of P8W48/rGO reveal a strong interaction between individual P8W48 and transparent rGO sheets. The calculation of the interaction between P8W48 and graphene (G) sheets is difficult to perform within a reasonable period of time because of the large size and very high overall negative charge of P8W48. However, as P8W48 is symmetrical, a quarter of its structure [H2P2W12O48](12-) (P2W12) was extracted as a DFT calculation model. As P8W48 in P8W48/rGO is neutral, due to surrounding counter cations, the calculation model P2W12 is neutral with protons considering the affordable computational time. The adsorption energy for P2W12 on G (-1.55 eV) and the charge transfer between P2W12 and G (0.66 vertical bar e vertical bar) indicate that a strong interaction between P2W12 and G sheets exists. Kinetic studies show that the P8W48/rGO hybrids display excellent HER activity in acid, further confirmed by reproducible generation of hydrogen with quantitative faradaic yield and a high turnover frequency (11 s(-1) at 295 mV overpotential) for a noble metal-free electrocatalyst. Importantly, the overpotentials required for the HER compare well with those of the commercial Pt/C (20 wt% Pt), which indicates that P8W48/rGO is a promising cheap HER electrocatalyst. We demonstrate here the most convincing experimental evidence of the "microenvironment effect" on HER electrocatalysis by a polyoxometalate.
语种: 英语
内容类型: 期刊论文
URI标识: http://ir.iccas.ac.cn/handle/121111/35906
Appears in Collections:光化学实验室_期刊论文

Files in This Item:

There are no files associated with this item.


作者单位: 1.Chinese Acad Sci, Inst Proc Engn, Key Lab Green Proc & Engn, Beijing 100190, Peoples R China
2.Jacobs Univ Bremen, Dept Life Sci & Chem, POB 750 561, D-28725 Bremen, Germany
3.Florida State Univ, Dept Chem & Biochem, Tallahassee, FL 32306 USA
4.Chinese Acad Sci, Inst Chem, Key Lab Photochem, BNLMS, Beijing 100190, Peoples R China
5.Natl Ctr Nanosci & Technol, Key Lab Nanosyst & Hierarch Fabricat, Beijing 100190, Peoples R China
6.NE Normal Univ, Fac Chem, Changchun 130024, Peoples R China
7.Univ Paris 11, CNRS, UMR 8000, Chim Phys Lab, F-91405 Orsay, France
Service
Recommend this item
Sava as my favorate item
Show this item's statistics
Export Endnote File
Google Scholar
Similar articles in Google Scholar
[Liu, Rongji]'s Articles
[Zhang, Guangjin]'s Articles
[Cao, Hongbin]'s Articles
CSDL cross search
Similar articles in CSDL Cross Search
[Liu, Rongji]‘s Articles
[Zhang, Guangjin]‘s Articles
[Cao, Hongbin]‘s Articles
Related Copyright Policies
Null
Social Bookmarking
Add to CiteULike Add to Connotea Add to Del.icio.us Add to Digg Add to Reddit
所有评论 (0)
暂无评论
 
评注功能仅针对注册用户开放,请您登录
您对该条目有什么异议,请填写以下表单,管理员会尽快联系您。
内 容:
Email:  *
单位:
验证码:   刷新
您在IR的使用过程中有什么好的想法或者建议可以反馈给我们。
标 题:
 *
内 容:
Email:  *
验证码:   刷新

Items in IR are protected by copyright, with all rights reserved, unless otherwise indicated.

 

 

Valid XHTML 1.0!
Copyright © 2007-2017  中国科学院化学研究所 - Feedback
Powered by CSpace