MOF-Transformed In2O3-x@C Nanocorn Electrocatalyst for Efficient CO2 Reduction to HCOOH

Highlights The nanocorn design enables In 2 O 3- x @C a high Faradaic efficiency of 98% and a high formate current density of 320 mA cm −2 at a low potential of -1.2 V versus hydrogen electrode without iR correction. The rich O vacancy activates In 3+ sites on the nanocube shell of In 2 O 3- x @C an...

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Veröffentlicht in:Nano-Micro Letters 2022-12, Vol.14 (1), p.167, Article 167
Hauptverfasser: Qiu, Chen, Qian, Kun, Yu, Jun, Sun, Mingzi, Cao, Shoufu, Gao, Jinqiang, Yu, Rongxing, Fang, Lingzhe, Yao, Youwei, Lu, Xiaoqing, Li, Tao, Huang, Bolong, Yang, Shihe
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container_issue 1
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container_title Nano-Micro Letters
container_volume 14
creator Qiu, Chen
Qian, Kun
Yu, Jun
Sun, Mingzi
Cao, Shoufu
Gao, Jinqiang
Yu, Rongxing
Fang, Lingzhe
Yao, Youwei
Lu, Xiaoqing
Li, Tao
Huang, Bolong
Yang, Shihe
description Highlights The nanocorn design enables In 2 O 3- x @C a high Faradaic efficiency of 98% and a high formate current density of 320 mA cm −2 at a low potential of -1.2 V versus hydrogen electrode without iR correction. The rich O vacancy activates In 3+ sites on the nanocube shell of In 2 O 3- x @C and the carbon cob enhances conductivity. Operando X-ray absorption spectroscopy unveils the active site of In 3+ for formate production although reduction of In 3+ to In is conceivable at the applied negative potentials during CO 2 reduction reaction. For electrochemical CO 2 reduction to HCOOH, an ongoing challenge is to design energy efficient electrocatalysts that can deliver a high HCOOH current density ( J HCOOH ) at a low overpotential. Indium oxide is good HCOOH production catalyst but with low conductivity. In this work, we report a unique corn design of In 2 O 3- x @C nanocatalyst, wherein In 2 O 3- x nanocube as the fine grains dispersed uniformly on the carbon nanorod cob, resulting in the enhanced conductivity. Excellent performance is achieved with 84% Faradaic efficiency (FE) and 11 mA cm −2 J HCOOH at a low potential of − 0.4 V versus RHE. At the current density of 100 mA cm −2 , the applied potential remained stable for more than 120 h with the FE above 90%. Density functional theory calculations reveal that the abundant oxygen vacancy in In 2 O 3- x has exposed more In 3+ sites with activated electroactivity, which facilitates the formation of HCOO* intermediate. Operando X-ray absorption spectroscopy also confirms In 3+ as the active site and the key intermediate of HCOO* during the process of CO 2 reduction to HCOOH.
doi_str_mv 10.1007/s40820-022-00913-6
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The rich O vacancy activates In 3+ sites on the nanocube shell of In 2 O 3- x @C and the carbon cob enhances conductivity. Operando X-ray absorption spectroscopy unveils the active site of In 3+ for formate production although reduction of In 3+ to In is conceivable at the applied negative potentials during CO 2 reduction reaction. For electrochemical CO 2 reduction to HCOOH, an ongoing challenge is to design energy efficient electrocatalysts that can deliver a high HCOOH current density ( J HCOOH ) at a low overpotential. Indium oxide is good HCOOH production catalyst but with low conductivity. In this work, we report a unique corn design of In 2 O 3- x @C nanocatalyst, wherein In 2 O 3- x nanocube as the fine grains dispersed uniformly on the carbon nanorod cob, resulting in the enhanced conductivity. Excellent performance is achieved with 84% Faradaic efficiency (FE) and 11 mA cm −2 J HCOOH at a low potential of − 0.4 V versus RHE. At the current density of 100 mA cm −2 , the applied potential remained stable for more than 120 h with the FE above 90%. Density functional theory calculations reveal that the abundant oxygen vacancy in In 2 O 3- x has exposed more In 3+ sites with activated electroactivity, which facilitates the formation of HCOO* intermediate. 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The rich O vacancy activates In 3+ sites on the nanocube shell of In 2 O 3- x @C and the carbon cob enhances conductivity. Operando X-ray absorption spectroscopy unveils the active site of In 3+ for formate production although reduction of In 3+ to In is conceivable at the applied negative potentials during CO 2 reduction reaction. For electrochemical CO 2 reduction to HCOOH, an ongoing challenge is to design energy efficient electrocatalysts that can deliver a high HCOOH current density ( J HCOOH ) at a low overpotential. Indium oxide is good HCOOH production catalyst but with low conductivity. In this work, we report a unique corn design of In 2 O 3- x @C nanocatalyst, wherein In 2 O 3- x nanocube as the fine grains dispersed uniformly on the carbon nanorod cob, resulting in the enhanced conductivity. Excellent performance is achieved with 84% Faradaic efficiency (FE) and 11 mA cm −2 J HCOOH at a low potential of − 0.4 V versus RHE. At the current density of 100 mA cm −2 , the applied potential remained stable for more than 120 h with the FE above 90%. Density functional theory calculations reveal that the abundant oxygen vacancy in In 2 O 3- x has exposed more In 3+ sites with activated electroactivity, which facilitates the formation of HCOO* intermediate. Operando X-ray absorption spectroscopy also confirms In 3+ as the active site and the key intermediate of HCOO* during the process of CO 2 reduction to HCOOH.</abstract><cop>Singapore</cop><pub>Springer Nature Singapore</pub><pmid>35976472</pmid><doi>10.1007/s40820-022-00913-6</doi><oa>free_for_read</oa></addata></record>
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subjects Absorption spectroscopy
active sites
Carbon dioxide
Chemical reduction
CO2 reduction
corn design
Current density
Density functional theory
Electroactivity
Electrocatalysts
Electrocatalytic CO2 Reduction
Engineering
formate
indium oxide
Indium oxides
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Low conductivity
Nanorods
Nanoscale Science and Technology
Nanotechnology
Nanotechnology and Microengineering
Spectrum analysis
X ray absorption
title MOF-Transformed In2O3-x@C Nanocorn Electrocatalyst for Efficient CO2 Reduction to HCOOH
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