Yu Baiyang, Cheng Lu, Dai Sheng, Jiang Yongjun, Yang Bing, Li Hong, Zhao Yi, Xu Jing, Zhang Ying, Pan Chengsi, Cao Xiao-Ming, Zhu Yongfa, Lou Yang
Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi, Jiangsu, 214122, China.
International Joint Research Center for Photoresponsive Molecules and Materials, Jiangnan University, Wuxi, Jiangsu, 214122, China.
Adv Sci (Weinh). 2023 Sep;10(26):e2302143. doi: 10.1002/advs.202302143. Epub 2023 Jul 3.
Rationally constructing atom-precise active sites is highly important to promote their catalytic performance but still challenging. Herein, this work designs and constructs ZSM-5 supported Cu and Ag dual single atoms as a proof-of-concept catalyst (Ag -Cu /ZSM-5 hetero-SAC (single-atom catalyst)) to boost direct oxidation of methane (DOM) by H O . The Ag -Cu /ZSM-5 hetero-SAC synthesized via a modified co-adsorption strategy yields a methanol productivity of 20,115 µmol g with 81% selectivity at 70 °C within 30 min, which surpasses most of the state-of-the-art noble metal catalysts. The characterization results prove that the synergistic interaction between silver and copper facilitates the formation of highly reactive surface hydroxyl species to activate the C-H bond as well as the activity, selectivity, and stability of DOM compared with SACs, which is the key to the enhanced catalytic performance. This work believes the atomic-level design strategy on dual-single-atom active sites should pave the way to designing advanced catalysts for methane conversion.
合理构建原子精确的活性位点对于提升其催化性能至关重要，但仍具有挑战性。在此，本工作设计并构建了ZSM-5负载的铜和银双单原子作为概念验证催化剂（Ag-Cu/ZSM-5异质单原子催化剂），以促进甲烷（CH₄）被H₂O直接氧化（DOM）。通过改进的共吸附策略合成的Ag-Cu/ZSM-5异质单原子催化剂在70℃下30分钟内甲醇产率为20115 μmol g⁻¹，选择性为81%，超过了大多数现有最先进的贵金属催化剂。表征结果证明，与单原子催化剂相比，银和铜之间的协同相互作用促进了高活性表面羟基物种的形成，从而激活C-H键以及DOM的活性、选择性和稳定性，这是催化性能增强的关键。本工作认为双单原子活性位点的原子级设计策略应为设计用于甲烷转化的先进催化剂铺平道路。
