SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2022, Vol. 43 ›› Issue (3): 62-69.DOI: 10.1016/j.cjche.2021.11.018

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

Bo Wu1,2, Xing Yu1,2, Min Huang1,3, Liangshu Zhong1,3, Yuhan Sun1,3   

  1. 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:2022-04-28 Published:2022-03-28
  • 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.

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

Bo Wu1,2, Xing Yu1,2, Min Huang1,3, Liangshu Zhong1,3, Yuhan Sun1,3   

  1. 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
  • 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.

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

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