Yang Xiaoli, Duan Hongmin, Wang Ruifeng, Zhao Fengwang, Jin Fayi, Jiang Wei, Han Guangting, Guan Qingxin, Ben Haoxi
College of Textiles and Clothing, State Key Laboratory of BioFibers and Eco-textiles, Qingdao University, Qingdao 266071, China.
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Inorg Chem. 2023 Aug 21;62(33):13419-13427. doi: 10.1021/acs.inorgchem.3c01763. Epub 2023 Aug 8.
The utilization of Cu-based catalysts in CO conversion into valuable chemicals is of significant interest due to their potential in mitigating greenhouse gas emissions. However, the controllable design of Cu-based catalysts and the regulation of their mechanism remain challenging. In this study, a series of efficient Cu/L catalysts were prepared for this process, and the intrinsic influencing factors on the reaction routes were systematically revealed. Various techniques revealed that Cu particles in L-supported catalysts exhibited higher dispersion and formed Cu-O(OH)-K interfacial sites. However, with increasing Cu loading, the dispersion of Cu particles and the percentage of Cu-O(OH)-K interfaces decreased. Kinetic investigations revealed that the adsorption configuration and electronic structure of Cu species codetermined the reaction pathways and resulting selectivity. Cu/L catalysts possessing Cu-O(OH)-K interfaces and small particles demonstrated the preferential formation of formate species, promoting methanol formation. However, larger Cu particles generated carboxylate intermediates, resulting in higher CO selectivity..
由于铜基催化剂在减少温室气体排放方面的潜力,其在将CO转化为有价值化学品中的应用备受关注。然而,铜基催化剂的可控设计及其机理调控仍然具有挑战性。在本研究中,制备了一系列用于该过程的高效Cu/L催化剂,并系统地揭示了影响反应路径的内在因素。各种技术表明,负载在L上的催化剂中的铜颗粒表现出更高的分散性,并形成了Cu-O(OH)-K界面位点。然而,随着铜负载量的增加,铜颗粒的分散性和Cu-O(OH)-K界面的百分比降低。动力学研究表明,铜物种的吸附构型和电子结构共同决定了反应路径和产物选择性。具有Cu-O(OH)-K界面和小颗粒的Cu/L催化剂表现出优先形成甲酸盐物种,促进甲醇生成。然而,较大的铜颗粒产生羧酸盐中间体,导致CO选择性更高。