文献类型：期刊文献

英文题名：Enhanced Activity of C2N-Supported Single Co Atom Catalyst by Single Atom Promoter

作者：Zhong, Wenhui Zhang, Guozhen Zhang, Yachao Jia, Chuanyi Yang, Tongtong Ji, Shentong Prezhdo, Oleg V. Yuan, Jianyong Luo, Yi Jiang, Jun

第一作者：Zhong, Wenhui

通信作者：Jiang, J[1]

机构：[1]Guizhou Inst Technol, Sch Chem Engn, Guiyang 550003, Guizhou, Peoples R China;[2]Guizhou Educ Univ, Inst Appl Phys, Guizhou Prov Key Lab Computat Nanomat Sci, Guiyang 550018, Guizhou, Peoples R China;[3]Univ Sci & Technol China Hefei, Hefei Natl Lab Phys Sci Microscale, iChEM Collaborat Innovat Ctr Chem Energy Mat, CAS Ctr Excellence Nanosci,Sch Chem & Mat Sci, Hefei 230026, Anhui, Peoples R China;[4]Univ Southern Calif, Dept Chem, Los Angeles, CA 90089 USA;[5]East China Univ Sci & Technol, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China;[6]East China Univ Sci & Technol, Shanghai Key Lab Adv Polymer Mat, Sch Mat Sci & Engn, Shanghai 200237, Peoples R China

第一机构：贵州理工学院化学工程学院

通信机构：corresponding author), Univ Sci & Technol China Hefei, Hefei Natl Lab Phys Sci Microscale, iChEM Collaborat Innovat Ctr Chem Energy Mat, CAS Ctr Excellence Nanosci,Sch Chem & Mat Sci, Hefei 230026, Anhui, Peoples R China.

年份：2019

卷号：10

期号：22

起止页码：7009-7014

外文期刊名：JOURNAL OF PHYSICAL CHEMISTRY LETTERS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000497261200008)】；

基金：This work was financially supported by NSFC (No. 21963007, 21790351, 21703045, 21763008), MOST (2018YFA0208603, 2017YFA0303500), and the Excellent Innovation Scientific and Technological Talents of Guizhou Province (QJKY[2018]058, QJKY[2014]248). O.V.P acknowledges support of the US Department of Energy (grant no. DE-SC0014429).

语种：英文

外文关键词：Catalysts - Cobalt - Electronic states - Graphene

摘要：The remarkable chemical activity of metal single-atom catalysts (SACs) lies in their unique electronic states associated with the low-coordination nature of single-atom sites. Yet, electronic state manipulation normally requires direct contact with other atoms, which inevitably changes the low-coordination environment. Herein, we found by first-principle calculations that the activity of a Co SAC for HCOOH dehydrogenation is appreciably enhanced via electronic state manipulation by a noncontact single atom promoter. A Co atom and a Sn/Ge/Pb atom are anchored in the same cavity of a graphitic C2N monolayer. Surprisingly, the nonbonded promoter makes two far splitting spin states of Co almost degenerate via charge redistribution of C2N support. Further, the high-spin Co gives a remarkably low reaction barrier comparable to Pt or Pd catalysts. Our results demonstrate that the activity of a SAC can be tuned via a noncontact promoter, casting new insights into electronic state modulation of SACs on graphene-like support.