Rh single atoms embedded in CeO2 nanostructure boost CO2 hydrogenation to HCOOH

doi:10.1016/j.cjche.2021.11.018

中国化学工程学报 ›› 2022, Vol. 43 ›› Issue (3): 62-69.DOI: 10.1016/j.cjche.2021.11.018

Rh single atoms embedded in CeO₂ nanostructure boost CO₂ hydrogenation to HCOOH

Bo Wu^1,2, Xing Yu^1,2, Min Huang^1,3, Liangshu Zhong^1,3, Yuhan Sun^1,3

1. CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China;
2. University of Chinese Academy of Sciences, Beijing 100049, China;
3. School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China. China

收稿日期:2021-08-23 修回日期:2021-10-23 出版日期:2022-03-28 发布日期:2022-04-28
通讯作者: Liangshu Zhong,E-mail:zhongls@sari.ac.cn;Yuhan Sun,E-mail:sunyh@sari.ac.cn
基金资助:
This work was supported by Natural Science Foundation of China (91945301), Program of Shanghai Academic/Technology Research Leader (20XD1404000), Key Research Program of Frontier Sciences of the Chinese Academy of Sciences (QYZDB-SSW-SLH035), the "Transformational Technologies for Clean Energy and Demonstration" and Strategic Priority Research Program of CAS (XDA21020600) and the Youth Innovation Promotion Association of CAS.

Rh single atoms embedded in CeO₂ nanostructure boost CO₂ hydrogenation to HCOOH

Bo Wu^1,2, Xing Yu^1,2, Min Huang^1,3, Liangshu Zhong^1,3, Yuhan Sun^1,3

1. CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China;
2. University of Chinese Academy of Sciences, Beijing 100049, China;
3. School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China. China

Received:2021-08-23 Revised:2021-10-23 Online:2022-03-28 Published:2022-04-28
Contact: Liangshu Zhong,E-mail:zhongls@sari.ac.cn;Yuhan Sun,E-mail:sunyh@sari.ac.cn
Supported by:
This work was supported by Natural Science Foundation of China (91945301), Program of Shanghai Academic/Technology Research Leader (20XD1404000), Key Research Program of Frontier Sciences of the Chinese Academy of Sciences (QYZDB-SSW-SLH035), the "Transformational Technologies for Clean Energy and Demonstration" and Strategic Priority Research Program of CAS (XDA21020600) and the Youth Innovation Promotion Association of CAS.

摘要/Abstract

摘要： CO₂ hydrogenation to value-added chemicals is a promising pathway to solve CO₂-relevant environmental problems but still remains a great challenge. Herein, we report a CeO₂ nanostructure supported Rh single atoms (Rh-SAs/CeO₂) catalyst and was used for the efficient CO₂ hydrogenation to HCOOH. The Rh-SAs/CeO₂ exhibited high catalytic activity with turnover numbers (TON) up to 221 at 200 ℃, which was 4-fold to that of CeO₂ supported Rh nanoparticles (Rh-NPs/CeO₂). Moreover, HCOOH selectivity for Rh-SAs/CeO₂ reached 85%, much higher than that of Rh-NPs/CeO₂ (46%). Mechanism studies revealed that Rh single atoms in the Rh-SAs/CeO₂ with high metal atoms utilization efficiency not only provided abundant active sites to promote the catalytic activity, but also suppressed the decomposition of HCOOH to CO and benefited the formation of HCOOH.

关键词: CO₂ hydrogenation, Selectivity, Single-atom catalysts (SACs), Rh, HCOOH

Abstract: CO₂ hydrogenation to value-added chemicals is a promising pathway to solve CO₂-relevant environmental problems but still remains a great challenge. Herein, we report a CeO₂ nanostructure supported Rh single atoms (Rh-SAs/CeO₂) catalyst and was used for the efficient CO₂ hydrogenation to HCOOH. The Rh-SAs/CeO₂ exhibited high catalytic activity with turnover numbers (TON) up to 221 at 200 ℃, which was 4-fold to that of CeO₂ supported Rh nanoparticles (Rh-NPs/CeO₂). Moreover, HCOOH selectivity for Rh-SAs/CeO₂ reached 85%, much higher than that of Rh-NPs/CeO₂ (46%). Mechanism studies revealed that Rh single atoms in the Rh-SAs/CeO₂ with high metal atoms utilization efficiency not only provided abundant active sites to promote the catalytic activity, but also suppressed the decomposition of HCOOH to CO and benefited the formation of HCOOH.

Key words: CO₂ hydrogenation, Selectivity, Single-atom catalysts (SACs), Rh, HCOOH

Bo Wu, Xing Yu, Min Huang, Liangshu Zhong, Yuhan Sun. Rh single atoms embedded in CeO₂ nanostructure boost CO₂ hydrogenation to HCOOH[J]. 中国化学工程学报, 2022, 43(3): 62-69.

Bo Wu, Xing Yu, Min Huang, Liangshu Zhong, Yuhan Sun. Rh single atoms embedded in CeO₂ nanostructure boost CO₂ hydrogenation to HCOOH[J]. Chinese Journal of Chemical Engineering, 2022, 43(3): 62-69.

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Rh single atoms embedded in CeO₂ nanostructure boost CO₂ hydrogenation to HCOOH

Rh single atoms embedded in CeO₂ nanostructure boost CO₂ hydrogenation to HCOOH

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