Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation

Xiong, Yu; Dong, Juncai; Huang, Zheng-Qing; Xin, Pingyu; Chen, Wenxing; Wang, Yu; Li, Zhi; Jin, Zhao; Xing, Wei; Zhuang, Zhongbin; Ye, Jinyu; Wei, Xing; Cao, Rui; Gu, Lin; Sun, Shigang; Zhuang, Lin; Chen, Xiaoqing; Yang, Hua; Chen, Chen; Peng, Qing; Chang, Chun-Ran; Wang, Dingsheng; Li, Yadong

doi:10.1038/s41565-020-0665-x

Title: Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation

Journal Article · Mon Mar 30 00:00:00 EDT 2020 · Nature Nanotechnology

DOI:https://doi.org/10.1038/s41565-020-0665-x· OSTI ID:1616956

Xiong, Yu ^[1];

^[2];

^[3]; Xin, Pingyu ^[4]; Chen, Wenxing ^[4];

^[5]; Li, Zhi ^[4]; Jin, Zhao ^[6]; Xing, Wei ^[6]; Zhuang, Zhongbin ^[7];

^[8]; Wei, Xing ^[9];

^[10]; Gu, Lin ^[11]; Sun, Shigang ^[8];

^[9]; Chen, Xiaoqing ^[12]; Yang, Hua ^[12]; Chen, Chen ^[4]; Peng, Qing ^[4] more »

Tsinghua Univ., Beijing (China); Central South Univ., Changsha (China)
Chinese Academy of Sciences (CAS), Beijing (China). Inst. of High Energy Physics, Beijing Synchrotron Radiation Facility
Xi’an Jiaotong Univ. (China)
Tsinghua Univ., Beijing (China)
Chinese Academy of Science (CAS), Shanghai (China). Shanghai Inst. of Applied Physics, Shanghai Synchrotron Radiation Facilities
Chinese Academy of Sciences, Changchun (China). Changchun Inst. of Applied Chemistry; Jilin Province Key Lab. of Low Carbon Chemical Power Sources, Changchun (China)
Beijing Univ. of Chemical Technology (China)
Xiamen Univ. (China)
Wuhan Univ. (China)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics,
Central South Univ., Changsha (China)

To meet the requirements of potential applications, it is of great importance to explore new catalysts for formic acid oxidation that have both ultra-high mass activity and CO resistance. In this work, we successfully synthesize atomically dispersed Rh on N-doped carbon (SA-Rh/CN) and discover that SA-Rh/CN exhibits promising electrocatalytic properties for formic acid oxidation. The mass activity shows 28- and 67-fold enhancements compared with state-of-the-art Pd/C and Pt/C, respectively, despite the low activity of Rh/C. Interestingly, SA-Rh/CN exhibits greatly enhanced tolerance to CO poisoning, and Rh atoms in SA-Rh/CN resist sintering after long-term testing, resulting in excellent catalytic stability. Density functional theory calculations suggest that the formate route is more favourable on SA-Rh/CN. According to calculations, the high barrier to produce CO, together with the relatively unfavourable binding with CO, contribute to its CO tolerance.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Organization:: National Key Research and Development Program of China; National Natural Science Foundation of China (NSFC); China Postdoctoral Science Foundation; Jilin Province Science and Technology Development Program; USDOE Laboratory Directed Research and Development (LDRD) Program; Youth Innovation Promotion Association CAS

Grant/Contract Number:: AC02-76SF00515; 21671117; 21871159; 21890383

OSTI ID:: 1616956

Journal Information:: Nature Nanotechnology, Vol. 15, Issue 5; ISSN 1748-3387

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 256 works

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