A major challenge in the field of photocatalytic carbon dioxide (CO2) reduction is to design catalyst systems featuring high selectivity for CO production, long-term stability and a composition of Earth-abundant elements. Here, we present a metal-organic framework (MOF) based catalyst to mitigate the technical problems associated with the above-mentioned features. We report a carbon-coated CuNi alloy nanocatalyst obtained by high temperature vacuum treatment of a MOF material (CuNiBTC). The resulting carbon encapsulated CuNi (denoted as CuNi/C) nanoparticles possess a well-designed core-shell composite structure with graphene shells. Meanwhile, we investigated the reaction mechanism of CO2 on the surface of the CuNi/C photocatalyst in an aqueous solution containing triethanolamine. The experimental results show that the activity and catalytic yield of CuNi/C are much higher than those of Cu/C and Ni/C alone. At the same time, the catalytic activity of CuNi/C is also affected by changing the reaction temperature in the preparation process. As a result, the CuNi/C samples can achieve nearly 90% selectivity for NIR-light-driven CO2 reduction to CO. Our approach demonstrates the potential of non-semiconductor materials as catalysts for efficient and selective reduction of CO2 to CO.
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http://dx.doi.org/10.1039/c9dt04935e | DOI Listing |
J Am Chem Soc
January 2025
Department of Industrial and Systems Engineering, The Hong Kong Polytechnic University, Kowloon 999077, Hong Kong, China.
Palladium (Pd) catalysts are promising for electrochemical reduction of CO to CO but often can be deactivated by poisoning owing to the strong affinity of *CO on Pd sites. Theoretical investigations reveal that different configurations of *CO endow specific adsorption energies, thereby dictating the final performances. Here, a regulatory strategy toward *CO absorption configurations is proposed to alleviate CO poisoning by simultaneously incorporating Cu and Zn atoms into ultrathin Pd nanosheets (NSs).
View Article and Find Full Text PDFEnviron Sci Technol
January 2025
State Key Laboratory of Black Soils Conservation and Utilization, Northeast Institute of Geography and Agroecology, Chinese Academy of Sciences, Shengbei Street 4888, Changchun 130102, China.
Climate change and human activity are increasing the frequency of wildfires in peatlands and threatening permafrost peatland carbon pools. In Northeast China, low-severity prescribed fires are conducted annually on permafrost peatlands to reduce the risk of wildfires. These fires typically do not burn surface peat but lead to the loss of surface vegetation and introduction of pyrogenic carbon.
View Article and Find Full Text PDFSmall
January 2025
Environment Research Institute, Shandong University, Qingdao, 266237, China.
The direct electrochemical conversion of bicarbonate solutions (i.e., captured CO) has emerged as a sustainable approach for integrating CO capture and utilization compared to the traditional independent and sequential route.
View Article and Find Full Text PDFSmall
January 2025
School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an, 710049, China.
The photocatalytic conversion of CO into products such as CH and CH poses a significant challenge due to the lengthy reaction steps and the high energy barrier involved. In this study, both benzothiadiazole (BTD) and hydroxyl groups (-OH) are introduced into cobalt-based polymerized porphyrinic network (PPN) through a C-C coupling reaction. This modification of orbital energy levels that strengthens the ability of gain electrons and facilitates the charge transfer in PPN.
View Article and Find Full Text PDFACS Nano
January 2025
Songshan Lake Materials Laboratory (SLAB), Dongguan 523808, P. R. China.
Electrocatalytic CO reduction into high-value multicarbon products offers a sustainable approach to closing the anthropogenic carbon cycle and contributing to carbon neutrality, particularly when renewable electricity is used to power the reaction. However, the lack of efficient and durable electrocatalysts with high selectivity for multicarbons severely hinders the practical application of this promising technology. Herein, a nanoporous defective AuCu single-atom alloy (De-AuCu SAA) catalyst is developed through facile low-temperature thermal reduction in hydrogen and a subsequent dealloying process, which shows high selectivity toward ethylene (CH), with a Faradaic efficiency of 52% at the current density of 252 mA cm under a potential of -1.
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