Design and synthesis of thermally stable single atom catalysts for thermochemical CO2 reduction

doi:10.1016/j.jechem.2023.07.032

Journal of Energy Chemistry ›› 2023, Vol. 86 ›› Issue (11): 246-262.DOI: 10.1016/j.jechem.2023.07.032

Design and synthesis of thermally stable single atom catalysts for thermochemical CO₂ reduction

Eswaravara Prasadarao Komarala^a, Ayesha A. Alkhoori^a,b, Xiaolong Zhang^c, Hui-Ming Cheng^d,*, Kyriaki Polychronopoulou^a,b,*

^aDepartment of Mechanical Engineering, Khalifa University of Science and Technology, Main Campus, P.O. Box 127788, Abu Dhabi, United Arab Emirates;
^bCenter for Catalysis and Separations, Khalifa University of Science and Technology, P.O. Box 127788, Abu Dhabi, United Arab Emirates;
^cShenzhen Key Laboratory of Energy Materials for Carbon Neutrality, Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, Guangdong, China;
^dShenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, Liaoning, China

Received:2023-05-15 Revised:2023-07-05 Accepted:2023-07-06 Online:2023-11-15 Published:2023-11-07
Contact: *E-mail addresses: cheng@imr.ac.cn (H.-M. Cheng), kyriaki.polychrono@ku.ac.ae (K. Polychronopoulou).
About author:Eswaravara Prasadarao Komarala received his PhD from Indian Institute of Technology Bombay, India in 2017. He is currently working as a Post-Doctoral Fellow at Khalifa University of Science and Technology. His current research interests focus on development of supported nanohybrid materials for heterogeneous catalysis including CH₄ cracking and reforming, CO₂ conversion, H₂ production, and NH₃ synthesis and cracking reactions. He published over 25 papers and filed 4 US patents on GTL technology and NH₃ synthesis.
Ayesha A Alkhoori is a Materials Science and Engineering researcher. She obtained her PhD from Khalifa University of Science and Technology, UAE in 2023, where her academic excellence and innovative research were evident. Currently serving as a Post-Doctoral Fellow at RIC-2D in the same university, Ayesha's primary focus lies in the development of heterogeneous catalysts for CO₂ conversion. She was honored with the prestigious L'Oreal-UNESCO for women in science award in 2022. Additionally, in the same year, Ayesha was bestowed with the Outstanding Young Researcher Award and the Top Journal Publication Award by Khalifa University, further highlighting her significant impact in the research community.
Xiaolong Zhang received his PhD from Monash University under the supervision of Prof. Jie Zhang and Prof. Alan Bond in 2019. Then, he joined the Institute of Organic Chemistry at University of Münster, where he was a Postdoctoral Fellow supported by the Humboldt foundation in the group of Prof. Frank Glorius. Now, he is an Associated Professor at Shenzhen Institute of Advanced Technology. His research interests include CO₂ conversion, biomass upgrade conversion, and the utilization of other carbon resources.
Prof. Hui-Ming Cheng is the director of both the Advanced Carbon Research Division of Shenyang National Laboratory for Materials Science, Institute of Metal Research, CAS since 2001, and the Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, CAS since 2021. He is a member of CAS and a fellow of TWAS. His research activities mainly focus on energy materials and devices, carbon nanotubes, graphene, and other 2D materials. He published over 800 papers with an h-index of 158, and is a Highly Cited Researcher in three fields of materials science, chemistry, and environment and ecology. He has given over 230 plenary/keynote/invited lectures at various conferences, and won a few domestic and international awards. He is the founding Editor-in-Chief of Energy Storage Materials and has spun off several high-tech companies.
Prof. Kyriaki Polychronopoulou is a full professor at the Department of Mechanical Engineering and the founding Director of the Catalysis and Separation Center (CeCaS) at Khalifa University of Science and Technology. She is also a visiting Professor at ETH-Zurich. Her research centers on experimental and computational catalysis, exploring both fundamental and applied aspects. She aims to unravel reaction mechanisms and understand surface phenomena, particularly their connection to the microstructure of catalytic materials. Her primary focuses include H₂ production, CO₂ conversion, and biofuels production.

Abstract

Abstract: The continuous and excessive emission of CO₂ into the atmosphere presents a pressing challenge for global sustainable development. In response, researchers have been devoting significant efforts to develop methods for converting CO₂ into valuable chemicals and fuels. These conversions have the potential to establish a closed artificial carbon cycle and provide an alternative resource to depleting fossil fuels. Among the various conversion routes, thermochemical CO₂ reduction stands out as a promising candidate for industrialization. Within the realm of heterogeneous catalysis, single atom catalysts (SACs) have garnered significant attention. The utilization of SACs offers tremendous potential for enhancing catalytic performance. To achieve optimal activity and selectivity of SACs in CO₂ thermochemical reduction reactions, a comprehensive understanding of key factors such as single atom metal-support interactions, chemical coordination, and accessibility of active sites is crucial. Despite extensive research in this field, the atomic-scale reaction mechanisms in different chemical environments remain largely unexplored. While SACs have been found successful applications in electrochemical and photochemical CO₂ reduction reactions, their implementation in thermochemical CO₂ reduction encounters challenges due to the sintering and/or agglomeration effects that occur at elevated temperatures. In this review, we present a unique approach that combines theoretical understanding with experimental strategies to guide researchers in the design of controlled and thermally stable SACs. By elucidating the underlying principles, we aim to enable the creation of SACs that exhibit stable and efficient catalytic activity for thermochemical CO₂ reduction reactions. Subsequently, we provide a comprehensive overview of recent literature on noble metal- and transition metal-based SACs for thermochemical CO₂ reduction. The current review is focused on certain CO₂-derived products involving one step reduction only for simplicity and for better understanding the SACs enhancement mechanism. We emphasize various synthesis methods employed and highlight the catalytic activity of these SACs. Finally, we delve into the perspectives and challenges associated with SACs in the context of thermochemical CO₂ reduction reactions, providing valuable insights for future research endeavor. Through this review, we aim to contribute to the advancement of SACs in the field of thermochemical CO₂ reduction, shedding light on their potential as effective catalysts and addressing the challenges that need to be overcome for their successful implementation as paradigm shift in catalysis.

Key words: CO₂ utilization, CO₂ conversion, SACs, Added-value products, Thermochemical catalysis

Eswaravara Prasadarao Komarala, Ayesha A. Alkhoori, Xiaolong Zhang, Hui-Ming Cheng, Kyriaki Polychronopoulou. Design and synthesis of thermally stable single atom catalysts for thermochemical CO₂ reduction[J]. Journal of Energy Chemistry, 2023, 86(11): 246-262.

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Design and synthesis of thermally stable single atom catalysts for thermochemical CO₂ reduction

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