Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation
Abstract
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.
- Authors:
-
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- 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)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Sponsoring Org.:
- 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
- OSTI Identifier:
- 1616956
- Grant/Contract Number:
- AC02-76SF00515; 21671117; 21871159; 21890383
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Nanotechnology
- Additional Journal Information:
- Journal Volume: 15; Journal Issue: 5; Journal ID: ISSN 1748-3387
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Electrocatalysis; Materials science
Citation Formats
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, and Li, Yadong. Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation. United States: N. p., 2020.
Web. doi:10.1038/s41565-020-0665-x.
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. Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation. United States. https://doi.org/10.1038/s41565-020-0665-x
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, and Li, Yadong. Mon .
"Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation". United States. https://doi.org/10.1038/s41565-020-0665-x. https://www.osti.gov/servlets/purl/1616956.
@article{osti_1616956,
title = {Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation},
author = {Xiong, Yu and Dong, Juncai and Huang, Zheng-Qing and Xin, Pingyu and Chen, Wenxing and Wang, Yu and Li, Zhi and Jin, Zhao and Xing, Wei and Zhuang, Zhongbin and Ye, Jinyu and Wei, Xing and Cao, Rui and Gu, Lin and Sun, Shigang and Zhuang, Lin and Chen, Xiaoqing and Yang, Hua and Chen, Chen and Peng, Qing and Chang, Chun-Ran and Wang, Dingsheng and Li, Yadong},
abstractNote = {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.},
doi = {10.1038/s41565-020-0665-x},
journal = {Nature Nanotechnology},
number = 5,
volume = 15,
place = {United States},
year = {Mon Mar 30 00:00:00 EDT 2020},
month = {Mon Mar 30 00:00:00 EDT 2020}
}
Web of Science
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