电催化剂
过电位
法拉第效率
电化学
金属有机骨架
材料科学
卟啉
化学工程
选择性
无机化学
金属
X射线光电子能谱
催化作用
化学
电极
光化学
有机化学
冶金
吸附
物理化学
工程类
作者
Feroz Ahmad Sofi,Paras Kalra,Murtaza Manzoor Bhat,Adil Amin Wani,Sajad Ahmad Bhat,A. Bhat,Kowsar Majid,Pravin P. Ingole,Mohsin Ahmad Bhat
出处
期刊:ACS applied nano materials
[American Chemical Society]
日期:2023-10-23
卷期号:6 (21): 19689-19700
被引量:4
标识
DOI:10.1021/acsanm.3c03448
摘要
Cu-based metal–organic frameworks (MOFs) have emerged as promising modular materials for the design of electrochemically stable, efficient, and selective electrocatalysts for the electroreduction of carbon dioxide (ERCO2). Herein, we report the design and synthesis of a silver nanoparticle-decorated Cu-MOF-based tandem electrocatalyst that, besides its excellent electrochemical stability, exhibits excellent activity and selectivity toward electroreduction of CO2 to CH4. Specifically, the specially synthesized Cu(II) (metal) plus tetrakis(4-carboxyphenyl porphyrin) (TCPP-linker)-based 2D metal–organic frameworks (Cu-TCPP MOFs) were decorated with silver nanoparticles via a photoseeding approach for the fabrication of AgNP/Cu-TCPP MOFs. The coordination active sites of the as-designed AgNP/Cu-TCPP MOF composites were confirmed by XRD, FE-SEM, EDX, and XPS. Our results suggest that the anchoring of Ag NPs to Cu-TCPP MOFs, besides enhancing the electrochemical stability, significantly improves the electronic conductivity, electrocatalytic performance, and selectivity of these MOFs toward ERCO2. Importantly, the Ag-Np functionalization of Cu-TCPP MOF improves the Faradaic efficiency for CH4 from 5% (for the pristine MOF) to 73% while increasing the current density for CH4 production by a factor of 16 from 3 to 50 mA cm–2 and proportionately reducing the current density for CO and H2 production. With an overpotential of just ca. −1.378 V vs RHE, the AgNP/Cu-TCPP MOF exhibits a turnover number of 4 × 1022 cm–1 h–1 and turnover frequency of 1 × 104 h–1 (2.7 s–1) for CH4 production. The enhanced FE and selectivity of the tandem composite are attributed to the synergistic interaction between the atomically defined Cu sites and the Ag clusters in AgNP/Cu-TCPP MOFs.
科研通智能强力驱动
Strongly Powered by AbleSci AI