氮掺杂石墨烯包覆钴纳米核壳结构的双功能催化性能研究及其在锌空电池上的应用
详细信息    查看官网全文
摘要
石墨烯包覆的过渡金属纳米颗粒作为一种新型的电催化剂材料越来越受到人们的关注~([1-5])。研究者对这类石墨烯包覆的核壳结构提出了"电子注入"催化原理,认为内核的金属颗粒能够将电子注入到石墨烯壳层,从而改变外层石墨烯的功函数,使其成为催化的活性位点。本文介绍了以含钴普鲁士蓝类合物作为单一的前驱体,在氩气的保护下经过高温固相碳化反应,制备氮掺杂石墨烯包覆的钴纳米颗粒核壳结构(Co@NG),实验结果表明Co@NG在酸性和碱性溶液中都具备出色的电催化分解水析氢和氧还原性能,并且当大部分的内核钴纳米颗粒被HCl腐蚀掉以后,Co@NG-acid的催化活性并没有衰减,而是得到了进一步的提升,这也表明大部分的钴内核并没有直接参与电催化反应过程~([6])。我们进一步综合同步辐射、XPS、CN-离子的毒化测试结果提出该催化剂的活性位点是位于外层石墨烯壳层中间的微量Co-C-N结构。此外,我们将该催化剂应用到锌空电池的空气电极中,也表现出非常优异的功率密度和工作稳定性。
Transition metal nanoparticles encapsulated in graphene layers have emerged as a new type of functional materials and quickly attracted broad interest over recent years. In this study, we demonstrate that metallic cobalt nanoparticles sheathed by multilayered nitrogen-enriched graphene shells can be facilely prepared using cobalt-containing Prussian blue colloids as the single precursor. Co@NG exhibit great bifunctional activities for electrocatalytic oxygen reduction and hydrogen evolution in both alkaline and acidic electrolytes. Most importantly, after most of metallic cobalt cores leached out by HCl treatment, the performance of Co@NG-acid does not deteriorate but rather enhance. Based on this and other experimental observations, Co-N-C moieties are proposed as the catalytically active sites. At last, we show that these catalysts can be employed as the air catalyst of primary zinc-air batteries with excellent current density, power density and operation durability.
引文
[1]Deng,J.;Ren,P.;Deng,D.;Bao,X.;Angew.Chem.,Int.Ed.2015,54:2100.
    [2]Deng,D.;Yu,L.;Chen,X.;Wang,G.;Jin,L.;Pan,X.;Deng,J.;Sun,G.;Bao,X.;Angew.Chem.,Int.Ed.2013,52:371.
    [3]Deng,J.;Ren,P.;Deng,D.;Yu,L.;Yang,F.;Bao,X.;Energ.Environ.Sci.2014,7:1919.
    [4]Zou,X.;Huang,X.;Goswami,A.;Silva,R.;Sathe,B.;Mikmekova,E.;Asefa,T.;Angew.Chem.,Int.Ed.2014,53:4372.
    [5]Hu,Y.;Jensen,J.;Zhang,W.;Cleemann,L.;Xing,W.;Bjerrum,N.;Li,Q.;Angew.Chem.,Int.Ed.2014,53:3675.
    [6]Zeng,M.;Liu,Y.;Zhao,F.;Nie,K.;Han,N.;Wang,X.;Huang,W.;Song,X.;Zhong,J.;Li,G.;Adv.Funct.Mater.2016,in press.

© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号

地址:北京市海淀区学院路29号 邮编:100083

电话:办公室:(+86 10)66554848;文献借阅、咨询服务、科技查新:66554700