期刊
NANO LETTERS
卷 21, 期 9, 页码 4092-4098出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c01113
关键词
electrochemical CO2 reduction; palladium-copper alloy; two-dimensional nanodendrites; formate; stability
类别
资金
- Ministry of Science and Technology of China [2017YFA0204800]
- National Natural Science Foundation of China [21902114]
- Collaborative Innovation Center of Suzhou Nano Science and Technology
- 111 Project
- Joint International Research Laboratory of Carbon-Based Functional Materials and Devices
Alloying Pd with Cu in the form of two-dimensional nanodendrites enables highly stable and selective formate production, thanks to the combined electronic effect and nanostructuring effect, with remarkable catalytic performance under the working potential as cathodic as -0.4 V. This is rationalized by computational simulations showing that Cu atoms weaken the *CO adsorption and stabilize the *OCHO adsorption on neighboring Pd atoms.
Pd is the only metal that can catalyze electrochemical CO2 reduction to formate at close-to-zero overpotential. It is unfortunately subjected to severe poisoning by trace CO as the side product and suffers from deteriorating stability and selectivity with increasing overpotential. Here, we demonstrate that alloying Pd with Cu in the form of two-dimensional nanodendrites could enable highly stable and selective formate production. Such unique bimetallic nanostructures are formed as a result of the rapid in-plane growth and suppressed out-of-plane growth by carefully controlling a set of experimental parameters. Thanks to the combined electronic effect and nanostructuring effect, our alloy product catalyzes CO2 reduction to formate with remarkable stability and selectivity under the working potential as cathodic as -0.4 V. Our results are rationalized by computational simulations, evidencing that Cu atoms weaken the *CO adsorption and stabilize the *OCHO adsorption on neighboring Pd atoms.
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