Electrochemical CO2-to-Formate Conversion over Positive Charge Depleted Tin Sites

Rongcheng Peng; Yang Gao; Hussein A. Younus; Yan Zhang; Wenpeng Ni; Shiguo Zhang

doi:10.1021/acsaem.2c00504

Electrochemical CO₂-to-Formate Conversion over Positive Charge Depleted Tin Sites

Rongcheng Peng, Yang Gao, Hussein A. Younus, Yan Zhang^*, Wenpeng Ni^*, Shiguo Zhang^*

^*Corresponding author for this work

Nanotechnology Research Center

Research output: Contribution to journal › Article › peer-review

6 Citations (Scopus)

Abstract

Upgrading CO₂to formate systems is a promising avenue for fuel production, and SnO_xis a unique low-cost candidate for this conversion. However, the high oxygen affinity of Sn sites leads to a strong adsorption of O-bound intermediates, resulting in a low efficiency of CO₂reduction. Herein, density functional theory (DFT) calculations confirmed that a H-doping strategy of SnO₂produces partially depleted positive charge Sn sites, weakening the adsorption of HCOO∗ and boosting the electron transfer kinetics. Experimentally, H-doped commercial SnO₂nanoparticles (H-SnO₂) indeed had enhanced intrinsic activity for CO₂-to-formate conversion with suppressed hydrogen evolution performance. Remarkably, H-SnO₂achieves over 90.0% formate selectivity within -0.6 to -1.0 V (vs RHE) at the industrial current density of 220 mA cm^-2.

Original language	English
Pages (from-to)	9324-9332
Number of pages	9
Journal	ACS Applied Energy Materials
Volume	5
Issue number	8
DOIs	https://doi.org/10.1021/acsaem.2c00504
Publication status	Published - Aug 22 2022

Keywords

COelectrochemical reduction
formate production
hydrogen doping
positive charge depletion
tin oxide

ASJC Scopus subject areas

Chemical Engineering (miscellaneous)
Energy Engineering and Power Technology
Electrochemistry
Materials Chemistry
Electrical and Electronic Engineering

Access to Document

10.1021/acsaem.2c00504

Cite this

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title = "Electrochemical CO2-to-Formate Conversion over Positive Charge Depleted Tin Sites",

abstract = "Upgrading CO2to formate systems is a promising avenue for fuel production, and SnOxis a unique low-cost candidate for this conversion. However, the high oxygen affinity of Sn sites leads to a strong adsorption of O-bound intermediates, resulting in a low efficiency of CO2reduction. Herein, density functional theory (DFT) calculations confirmed that a H-doping strategy of SnO2produces partially depleted positive charge Sn sites, weakening the adsorption of HCOO∗ and boosting the electron transfer kinetics. Experimentally, H-doped commercial SnO2nanoparticles (H-SnO2) indeed had enhanced intrinsic activity for CO2-to-formate conversion with suppressed hydrogen evolution performance. Remarkably, H-SnO2achieves over 90.0% formate selectivity within -0.6 to -1.0 V (vs RHE) at the industrial current density of 220 mA cm-2.",

keywords = "COelectrochemical reduction, formate production, hydrogen doping, positive charge depletion, tin oxide",

author = "Rongcheng Peng and Yang Gao and Younus, {Hussein A.} and Yan Zhang and Wenpeng Ni and Shiguo Zhang",

year = "2022",

month = aug,

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doi = "10.1021/acsaem.2c00504",

language = "English",

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journal = "ACS Applied Energy Materials",

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T1 - Electrochemical CO2-to-Formate Conversion over Positive Charge Depleted Tin Sites

AU - Peng, Rongcheng

AU - Gao, Yang

AU - Younus, Hussein A.

AU - Zhang, Yan

AU - Ni, Wenpeng

AU - Zhang, Shiguo

PY - 2022/8/22

Y1 - 2022/8/22

N2 - Upgrading CO2to formate systems is a promising avenue for fuel production, and SnOxis a unique low-cost candidate for this conversion. However, the high oxygen affinity of Sn sites leads to a strong adsorption of O-bound intermediates, resulting in a low efficiency of CO2reduction. Herein, density functional theory (DFT) calculations confirmed that a H-doping strategy of SnO2produces partially depleted positive charge Sn sites, weakening the adsorption of HCOO∗ and boosting the electron transfer kinetics. Experimentally, H-doped commercial SnO2nanoparticles (H-SnO2) indeed had enhanced intrinsic activity for CO2-to-formate conversion with suppressed hydrogen evolution performance. Remarkably, H-SnO2achieves over 90.0% formate selectivity within -0.6 to -1.0 V (vs RHE) at the industrial current density of 220 mA cm-2.

AB - Upgrading CO2to formate systems is a promising avenue for fuel production, and SnOxis a unique low-cost candidate for this conversion. However, the high oxygen affinity of Sn sites leads to a strong adsorption of O-bound intermediates, resulting in a low efficiency of CO2reduction. Herein, density functional theory (DFT) calculations confirmed that a H-doping strategy of SnO2produces partially depleted positive charge Sn sites, weakening the adsorption of HCOO∗ and boosting the electron transfer kinetics. Experimentally, H-doped commercial SnO2nanoparticles (H-SnO2) indeed had enhanced intrinsic activity for CO2-to-formate conversion with suppressed hydrogen evolution performance. Remarkably, H-SnO2achieves over 90.0% formate selectivity within -0.6 to -1.0 V (vs RHE) at the industrial current density of 220 mA cm-2.

KW - COelectrochemical reduction

KW - formate production

KW - hydrogen doping

KW - positive charge depletion

KW - tin oxide

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