材料科学
吸附
催化作用
氧气
介孔材料
化学工程
氧化物
表面工程
纳米技术
化学物理
物理化学
化学
有机化学
工程类
冶金
作者
Fuping Pan,Xinyi Duan,Lingzhe Fang,Haoyang Li,Chao Wang,Yudong Wang,Teng Wang,Tao Li,Zhiyao Duan,Kaijie Chen
标识
DOI:10.1002/aenm.202303118
摘要
Abstract CO 2 reduction is a highly attractive route to transform CO 2 into useful feedstocks, of which C 2 products are more desired than C 1 , yet face high kinetic barriers of C−C electrocoupling. Here, the engineering of pore‐enabled local confinement reaction environments is reported for tuning the enrichment of surface‐adsorbed oxygen‐relevant species and the establishment of their pronounced benefits in promoting C−C coupling over oxide‐derived Cu‐based catalysts. A new approach of utilizing the microphase separation of a block copolymer is developed to fabricate bicontinuous mesoporous CuO nanofibers (CuO‐BPNF). The enhanced confinement from long‐range mesochannels enables the adsorption of OH ad /O ad on the Cu surface at a wide negative potential range of −0.7 – −1.3 V in CO 2 reduction, which cannot be achieved over conventional deficient and short‐range pores. Constant‐potential DFT calculations reveal that the surface‐bound oxygen species weakens *CO affinity with the Cu (111) surface and lowers the kinetic barriers for both *CO−CO dimerization and *CO hydrogenation to enable *CO−CHO coupling. Accordingly, a CO 2 ‐to‐C 2 Faradaic efficiency of 74.7% over CuO‐BPNF is shown, significantly larger than counterparts with conventional pores. This work offers a general design principle of confinement engineering to manage the adsorption of reactive species for steering reaction pathways in interfacial catalysis.
科研通智能强力驱动
Strongly Powered by AbleSci AI