Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation.,Nature Nanotechnology

当前位置： X-MOL 学术 › Nat. Nanotechnol. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation.
Nature Nanotechnology ( IF 38.1 ) Pub Date : 2020-03-30 , DOI: 10.1038/s41565-020-0665-x
Yu Xiong _{1,

2} , Juncai Dong ₃ , Zheng-Qing Huang ₄ , Pingyu Xin ₁ , Wenxing Chen ₁ , Yu Wang ₅ , Zhi Li ₁ , Zhao Jin _{6,

7} , Wei Xing _{6,

7} , Zhongbin Zhuang ₈ , Jinyu Ye ₉ , Xing Wei ₁₀ , Rui Cao ₁₁ , Lin Gu ₁₂ , Shigang Sun ₉ , Lin Zhuang ₁₀ , Xiaoqing Chen ₂ , Hua Yang ₂ , Chen Chen ₁ , Qing Peng ₁ , Chun-Ran Chang ₄ , Dingsheng Wang ₁ , Yadong Li ₁

Affiliation

Department of Chemistry, Tsinghua University, Beijing, China.
College of Chemistry and Chemical Engineering, Central South University, Changsha, Hunan, China.
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China.
Shaanxi Key Laboratory of Energy Chemical Process Intensification, School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an, China.
Shanghai Synchrotron Radiation Facilities, Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai, China.
Laboratory of Advanced Power Sources, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, Jilin, China.
Jilin Province Key Laboratory of Low Carbon Chemical Power Sources, Changchun, Jilin, China.
State Key Lab of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China.
State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, China.
College of Chemistry and Molecular Sciences, Hubei Key Lab of Electrochemical Power Sources, Wuhan University, Wuhan, China.
Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, USA.
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 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. Here, 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.

中文翻译：

用于甲酸氧化的单原子Rh / N掺杂碳电催化剂。

为了满足潜在应用的要求，探索具有超高质量活性和抗CO的新的甲酸氧化催化剂非常重要。在这里，我们成功地在N掺杂碳（SA-Rh / CN）上合成了原子分散的Rh，并发现SA-Rh / CN对甲酸氧化表现出有希望的电催化性能。尽管Rh / C的活性较低，但与现有的Pd / C和Pt / C相比，其质量活性分别提高了28倍和67倍。有趣的是，SA-Rh / CN对CO中毒的耐受性大大增强，并且SA-Rh / CN中的Rh原子经过长期测试后仍能抵抗烧结，从而具有出色的催化稳定性。密度泛函理论计算表明，甲酸盐途径在SA-Rh / CN上更有利。根据计算，

更新日期：2020-03-30

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南