A collaborative study led by Shanghai Jiao Tong University Global College（SJTUGC, abbreviated as GC）Associate Professor Yulian He and Distinguished Professor Xue-Qing Gong from the School of Chemistry and Chemical Engineering, has been published in the Journal of the American Chemical Society (JACS). The paper, titled “Ambient-Pressure C–C Coupling of CO2 Hydrogenation by NiFe/TiO2 Bimetallic Catalyst”, elucidates a reaction mechanism in which lattice oxygen and NiFe bimetallic sites synergistically promote the ambient-pressure hydrogenation of CO2 into C2–C3 hydrocarbons, primarily ethane. GC doctoral student Mingxin Jiang and Associate Professor Zhi-Qiang Wang from East China University of Science and Technology are co-first authors of the paper. Associate Professor Yulian He and Professor Xue-Qing Gong are the co-corresponding authors.
Considering further incorporation of distributed small-scale electrolytic H2 synthesis strategies operating at ambient to low pressures for greener production, the catalytic hydrogenation of CO2 to value-added C2+ products at ambient pressure offers promising solutions to trim carbon emissions with additional economic benefits. However, ambient-pressure synthesis of the C–C bond from CO2 hydrogenation is significantly constrained by Le Chatelier’s principle, leading to the dominant formation of CO byproduct (over 90%) via the reverse water–gas shift (RWGS) reaction. Developing ambient-pressure catalytic systems for CcC coupling is not simply a case of re-engineering the high-pressure systems for low-pressure operations, but instead requires extra precautions in the intricate design of catalysts specifically tailor-made for ambient-pressure conditions.
To address these challenges, the research team developed a NiFe/TiO2 catalyst capable of modulating the amount of lattice oxygen in the active sites by adjusting the H2 reduction temperature, thereby exhibiting tunable ambient-pressure C–C coupling performance. An optimal performance was achieved after reducing NiFe/TiO2 at 350 °C (NiFe-350/TiO2), yielding 27.8% CO2 conversion and 33.9% selectivity to C2–C3 hydrocarbon (primarily ethane) at 350 °C under atmospheric pressure, while significantly suppressing CO as a byproduct. In contrast, the catalyst reduced at 600 °C (NiFe-600/TiO2) showed almost no ambient-pressure C–C coupling performance.
Combinatorial studies employing in situ characterizations, kinetic, intermediate control experiments and first-principles calculations indicate the formation of partially oxidized Niδ+–O–Feδ+ in NiFe-350/TiO2, the dual-site synergy of which enhances CO2 activation and facilitates H2 heterolytic activation into Hδ− species that selectively hydrogenate *CO2 into HCOO* and *CH3O intermediates, thus suppressing CO by-product formation and resulting in effective ambient-pressure C–C coupling likely via an asymmetric *CH2–CH3 coupling mechanism. In stark contrast, the fully reduced NiFe bimetallic catalyst (NiFe-600/TiO2) favors a direct CO2 dissociation pathway instead to form *CO that easily desorbs from the surface, as well as homolytic H2 activation such that the C–C coupling process is unfavored.
The published research work reports the ambient–pressure synthesis of C2–C3 paraffins from direct CO2 hydrogenation and provides design rationales for efficient carbon chain propagation.
First Author Biography
Mingxin Jiang is a Ph.D. candidate (Class of 2025) at the Global College, Shanghai Jiao Tong University. He has been awarded the Best Poster Presentation Award at ICCN-2025. His research focuses on the rational design of catalysts for CO2 hydrogenation reactions.
Zhi-Qiang Wang is an Associate Professor and Master’s Supervisor at East China University of Science and Technology. His research focuses on heterogeneous theoretical catalysis and computation, particularly on the selective hydrogenation at metal oxide surfaces and interfaces. His work primarily centers on precise construction of metal oxide surface/interface structures, development of new catalytic theories for active hydrogen species, and exploration of emerging applications of multisource hydride species. To date, he has published nearly 60 SCI papers as first or corresponding author (including co-authorship), in internationally recognized journals such as Nature Communications (5), Journal of the American Chemical Society (3), ACS Catalysis (8), and Chemical Science (1). His publications have received over 4,000 citations, with an H-index of 35. He has presided over six research projects, including the National Natural Science Foundation of China (NSFC) General Program, NSFC Young Scientists Fund, and the Shanghai Super Postdoctoral Program. He also serves as the theoretical PI for a Young Scientist Project under the National Key R&D Program of China.
Corresponding Author Biography
Yulian He is an Associate Professor jointly appointed by the Global College and the School of Chemistry and Chemical Engineering at Shanghai Jiao Tong University, and serves as a doctoral advisor and the principal investigator of the Catalysis and AI Laboratory. Her research focuses on integrated experimental–theoretical–AI approaches to heterogeneous catalysis. Professor He received her B.S. degree from the College of Chemistry at Nankai University, and her Ph.D. degree from Yale University. She then conducted postdoctoral research at Stanford University. She has been recognized as a recipient of the Shanghai Sailing Program and the Shanghai Leading Talent Program (Overseas Category). To date, Professor He has published over 40 research articles in internationally renowned journals and contributed to four book chapters. She currently serves as a young editorial board member for multiple academic journals. Her research has been supported by the National Natural Science Foundation of China (NSFC), National Development and Reform Commission, Ministry of Science and Technology, Shanghai Science and Technology Commission, Chinese Academy of Sciences, and Contemporary Amperex Technology Co., Limited (CATL), among others. For more details, please visit her group website: https://sites.gc.sjtu.edu.cn/yulian-he/
Xue-Qing Gong is a Professor, Doctoral Advisor, and Chair of the Department of Chemical Engineering at the School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University. He is a recipient of the National Science Fund for Distinguished Young Scholars. His research focuses on theoretical catalysis and computational chemistry, with emphasis on both fundamental scientific issues, such as the catalytic mechanisms on surfaces of catalytic materials, surface structures of metal oxides, the thermodynamics and kinetics of surface adsorption and migration processes, and applied challenges related to the design of catalytic materials and process optimization in energy and environmental catalysis. He has also made significant contributions to the development of first-principles methods augmented by intelligent algorithms, particularly the application of artificial intelligence (AI) in spectroscopy analysis, material structure prediction, and reaction mechanism studies. His team has elucidated the dynamic and selective electron reservoir effect of rare earth elements in catalysis and developed a series of efficient descriptors for performance screening and optimization of thermal, photo-, and electrocatalytic materials in key catalytic reactions. Professor Gong has published over 300 SCI-indexed papers, including articles in Science (2), Nature Materials (1), Nature Chemistry (1), Physical Review Letters (5), Journal of the American Chemical Society (12), Angewandte Chemie-Internation Edition (12), Nature Communications (13), PNAS (1), and ACS Catalysis (18). His work has been cited over 15,000 times, and he has an H-index of 71. He has led numerous research projects funded by the National Natural Science Foundation of China (including Distinguished and Excellent Young Scholars and General Programs), the National Key R&D Program, the Shanghai Science and Technology Commission (including the Leading Academic Talent Program, Morning Star Program, and Dawn Program), and was appointed as an “Oriental Scholar” Distinguished Professor in Shanghai. As a key contributor, he received the Second Prize of the Ministry of Education’s Higher Education Scientific Research Outstanding Achievement Award (Science and Technology) in 2019 (5th of 7 authors), and the Second Prize of the Shanghai Science and Technology Award (Natural Science) in 2022 and 2023 (2nd of 4 authors and 4th of 5 authors, respectively). He has served as an Editorial Board Member of the Journal of Fuel Chemistry and Technology since 2020 and was elected a Committee Member of the Theoretical Chemistry Division of the Chinese Chemical Society in 2022.
