Siqi Li, Yuda Zhang, Qiang Guo, Yafei Liang, Yuji Qi, Xiaowei Zhao, Yehong Wang*, Feng Wang
Chem. Eng. J., 2025, 508, 161144
The ethanol dehydrogenation condensation to ethyl acetate is a promising pathway, however, limited to low ethyl acetate selectivity due to the various side-reactions catalyzed by acid-base sites. Here, an efficient CuZnZrO solid solution catalyst was developed, and a superior ethyl acetate selectivity of 95.7% was achieved with a comparable ethanol conversion of 50.3%. The balance of acid-base aroused from zinc (Zn) doping into the CuZrO matrix contributed to its excellent catalytic performance. It was also noteworthy that the result of ∼2200 h life-test suggested a remarkable stability of CuZnZrO solid solution catalyst. This work offers a highly efficient catalytic system for the selective production of ethyl acetate from ethanol.
Xueyuan Wang, Xueshang Xin, Lunqiao Xiong, Jianlong Yang, Tieou Wang, Yang Yang, Zhipeng Huang, Nengchao Luo*, Junwang Tang*, Feng Wang
Angew. Chem. Int. Ed., 2025, DOI: 10.1002/anie.202420606
Hydroxy radical (•OH) is a prestigious oxidant that allows the cleavage of strong chemical bonds of methane but is untamed, leading to over-oxidation of methane and waste of oxidants, especially at high methane conversion. Here, we managed to buffer •OH in an aqueous solution of photo-irradiated Fe3+, where •OH almost participates in methane oxidation. Due to the interaction between Fe3+ and SO42−, the electron transfer from OH− to excited-state Fe3+ for •OH generation is retarded, while excessive •OH is consumed by generated Fe2+ to restore Fe3+. When combined with a Ru/SrTiO3:Rh photocatalyst, the buffered •OH converts methane to C2+ hydrocarbons and H2 with formation rates of 246 and 418 μmol h−1, respectively. The apparent quantum efficiency reaches 13.0 ± 0.2%, along with 10.2% methane conversion and 81% C2+ selectivity after 80 hours of reaction. Overall, this work presents a strategy for controlling active radicals for selective and efficient photocatalysis.
Ping Wu, Fangming Du, Qiang Xue, Hanxi Li, Ming-Chen Fu, Xukai Zhou,* and Feng Wang
Adv. Funct. Mater. 2025, 2420941. (DOI: 10.1002/adfm.202420941)
In this paper, three gold(I) cyclic trinuclear complexes (Au-CTCs) based metal–organic frameworks (MOFs) are prepared, exhibiting good photothermal conversion efficiency and H2O2 evolution rates. The production rates of H₂O₂ can reach as high as 51,987 µm g⁻¹ h⁻¹, surpassing the performance of most reported MOFs. The thermal-assisted photocatalytic mechanism is comprehensively studied by transient photocurrent response, electrochemical impedance, electron paramagnetic resonance, rotating ring disk electrode test and among others, demonstrating thermal energy can enhance the mobility of photogenerated carriers and apparent quantum yield, regulate the reactive species ratio and H2O2 selectivity, reduce the apparent activation energy of photocatalysis, and improve mass transfer rates, thereby accelerating the reaction process. This study offers new insights into the thermal-assisted photocatalytic production of H2O2.
Hao Han+, Qiang Xue+, Jiehua Ding, Jianyu Han, Hanxi Li, Yougui Li,* Xukai Zhou*
ACS Appl. Polym. Mater. 2025, 7, 3, 1338–1346. (DOI: 10.1021/acsapm.4c03047)
The classical organic dyes anthracene, acridine, and phenazine, as building blocks in the construction of three covalent organic frameworks (COFs), are presented for comprehensive comparison studies. Employing a sophisticated atomic-level skeleton-editing strategy through the precise adjustment of nitrogen content enables the regulation of intrinsic properties across macro- to micro-scales. In application experiments, photocatalytic hydrogen evolution (PHE) is studied as a model reaction. The results suggest that the anthracene-based COF (COF-Ant), with the strongest electron-donating ability, achieves the highest PHE rate among the three COFs at 2493 μmol·g–1·h–1. Additionally, the uniformity of the three COFs is highlighted, including shared features such as organic dyes and imine linkages, resulting in wide visible absorption, a narrow band gap, and topological features.