Searching for an efficient single-atom catalyst for benzene hydroxylation to phenol is of critical importance, but it still remains a challenge. Herein, a single-atom catalyst with unique Cu-N moieties (Cu-N/HCNS) was prepared and confirmed by HAADF-STEM and EXAFS. Turnover number (TON) over Cu-N/HCNS (6,935) is 3.4 times of Cu-N/HCNS (2,034) under the same reaction conditions, and both exhibit much higher phenol selectivity (close to 99%) and stability compared with Cu nanoparticles and nanoclusters. Experiments and DFT calculations reveal that atomically dispersed Cu species are active sites for benzene hydroxylation to phenol, and the Cu-N is more active than Cu-N owing to its much lower energy barrier concerning the activation of HO led by its unique coordination state of local atomic structure. We envision that this work opens a new window for modulating coordination environments of single metallic atoms in catalysis design.
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http://dx.doi.org/10.1016/j.isci.2019.11.010 | DOI Listing |
J Environ Sci (China)
July 2025
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China; University of Chinese Academy of Sciences, Beijing 100049, China. Electronic address:
Formamide condensation with Ni can generate the NC structure, widely recognized as an efficient catalyst for electrocatalytic CO reduction reaction (CORR). To improve the utilization efficiency of Ni atoms, we introduced metal oxides as substrates to modulate the growth of a formamide-Ni (FA-Ni) condensate. FA-Ni@TiO demonstrated 2.
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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 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.
View Article and Find Full Text PDFChemSusChem
January 2025
Osaka University: Osaka Daigaku, Research Center for Solar Energy Chemistry, 1-3 Machikaneyama, Toyonaka, 560-8531, Osaka, JAPAN.
Electrochemically grown copper nanoclusters (CuNCs: < 3 nm) from single-atom catalysts have recently attracted intensive attention as electrocatalysts for CO2 and CO reduction reaction (CO2RR/CORR) because they exhibit distinct product selectivity compared with conventional Cu nanoparticles (typically larger than 10 nm). Herein, we conducted a detailed investigation into the size dependence of CuNCs on selectivity for multicarbon (C2+) production in CORR. These nanoclusters were electrochemically grown from single Cu atoms dispersed on covalent triazine frameworks (Cu-CTFs).
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January 2025
CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
Single-atom catalysts (SACs) with unique geometric and electronic configurations have triggered great interest in many important reactions. However, controllably modulating the electronic structure of metal centers to enhance catalytic performance remains a challenge. Here, the electronic structure of Ni centers over Ni-NC SACs by introducing electron-rich phosphorus or electron-deficient boron for electrochemical CO reduction (CORR) is systematically tailored.
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