Rational design of asymmetric atomic Ni-P1N3 active sites for promoting electrochemical CO2 reduction

Ming Qu; Zhe Chen; Zhiyi Sun; Danni Zhou; Wenjing Xu; Hao Tang; Hongfei Gu; Tuo Liang; Pengfei Hu; Guangwen Li; Yu Wang; Zhuo Chen; Tao Wang; Binbin Jia

doi:10.1007/s12274-022-4969-z

Rational design of asymmetric atomic Ni-P₁N₃ active sites for promoting electrochemical CO₂ reduction

Ming Qu, Zhe Chen, Zhiyi Sun, Danni Zhou, Wenjing Xu, Hao Tang, Hongfei Gu, Tuo Liang, Pengfei Hu, Guangwen Li, Yu Wang, Zhuo Chen^*, Tao Wang^*, Binbin Jia^*

^*Corresponding author for this work

School of Material Science and Engineering

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

40 Citations (Scopus)

Abstract

The atomic-level interfacial regulation of single metal sites through heteroatom doping can significantly improve the characteristics of the catalyst and obtain surprising activity. Herein, nickel single-site catalysts (SSCs) with dual-coordinated phosphorus and nitrogen atoms were developed and confirmed (denoted as Ni-P_xN_y, x = 1, 2 and y = 3, 2). In CO₂ reduction reaction (CO₂RR), the CO current density on Ni-P_xN_y was significantly higher than that of Ni-N₄ catalyst without phosphorus modification. Besides, Ni-P₁N₃ performed the highest CO Faradaic efficiency (FE_CO) of 85.0%–98.0% over a wide potential range of −0.65 to −0.95 V (vs. the reversible hydrogen electrode (RHE)). Experimental and theoretical results revealed that the asymmetric Ni-P₁N₃ site was beneficial to CO₂ intermediate adsorption/desorption, thereby accelerating the reaction kinetics and boosting CO₂RR activity. This work provides an effective method for preparing well-defined dual-coordinated SSCs to improve catalytic performance, targetting to CO₂RR applications. [Figure not available: see fulltext.]

Original language	English
Pages (from-to)	2170-2176
Number of pages	7
Journal	Nano Research
Volume	16
Issue number	2
DOIs	https://doi.org/10.1007/s12274-022-4969-z
Publication status	Published - Feb 2023

Keywords

CO reduction reaction
asymmetric coordination
atomic interface
nickel single-site catalysts

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title = "Rational design of asymmetric atomic Ni-P1N3 active sites for promoting electrochemical CO2 reduction",

abstract = "The atomic-level interfacial regulation of single metal sites through heteroatom doping can significantly improve the characteristics of the catalyst and obtain surprising activity. Herein, nickel single-site catalysts (SSCs) with dual-coordinated phosphorus and nitrogen atoms were developed and confirmed (denoted as Ni-PxNy, x = 1, 2 and y = 3, 2). In CO2 reduction reaction (CO2RR), the CO current density on Ni-PxNy was significantly higher than that of Ni-N4 catalyst without phosphorus modification. Besides, Ni-P1N3 performed the highest CO Faradaic efficiency (FECO) of 85.0%–98.0% over a wide potential range of −0.65 to −0.95 V (vs. the reversible hydrogen electrode (RHE)). Experimental and theoretical results revealed that the asymmetric Ni-P1N3 site was beneficial to CO2 intermediate adsorption/desorption, thereby accelerating the reaction kinetics and boosting CO2RR activity. This work provides an effective method for preparing well-defined dual-coordinated SSCs to improve catalytic performance, targetting to CO2RR applications. [Figure not available: see fulltext.]",

keywords = "CO reduction reaction, asymmetric coordination, atomic interface, nickel single-site catalysts",

author = "Ming Qu and Zhe Chen and Zhiyi Sun and Danni Zhou and Wenjing Xu and Hao Tang and Hongfei Gu and Tuo Liang and Pengfei Hu and Guangwen Li and Yu Wang and Zhuo Chen and Tao Wang and Binbin Jia",

note = "Publisher Copyright: {\textcopyright} 2022, Tsinghua University Press.",

year = "2023",

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doi = "10.1007/s12274-022-4969-z",

language = "English",

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TY - JOUR

T1 - Rational design of asymmetric atomic Ni-P1N3 active sites for promoting electrochemical CO2 reduction

AU - Qu, Ming

AU - Chen, Zhe

AU - Sun, Zhiyi

AU - Zhou, Danni

AU - Xu, Wenjing

AU - Tang, Hao

AU - Gu, Hongfei

AU - Liang, Tuo

AU - Hu, Pengfei

AU - Li, Guangwen

AU - Wang, Yu

AU - Chen, Zhuo

AU - Wang, Tao

AU - Jia, Binbin

PY - 2023/2

Y1 - 2023/2

N2 - The atomic-level interfacial regulation of single metal sites through heteroatom doping can significantly improve the characteristics of the catalyst and obtain surprising activity. Herein, nickel single-site catalysts (SSCs) with dual-coordinated phosphorus and nitrogen atoms were developed and confirmed (denoted as Ni-PxNy, x = 1, 2 and y = 3, 2). In CO2 reduction reaction (CO2RR), the CO current density on Ni-PxNy was significantly higher than that of Ni-N4 catalyst without phosphorus modification. Besides, Ni-P1N3 performed the highest CO Faradaic efficiency (FECO) of 85.0%–98.0% over a wide potential range of −0.65 to −0.95 V (vs. the reversible hydrogen electrode (RHE)). Experimental and theoretical results revealed that the asymmetric Ni-P1N3 site was beneficial to CO2 intermediate adsorption/desorption, thereby accelerating the reaction kinetics and boosting CO2RR activity. This work provides an effective method for preparing well-defined dual-coordinated SSCs to improve catalytic performance, targetting to CO2RR applications. [Figure not available: see fulltext.]

AB - The atomic-level interfacial regulation of single metal sites through heteroatom doping can significantly improve the characteristics of the catalyst and obtain surprising activity. Herein, nickel single-site catalysts (SSCs) with dual-coordinated phosphorus and nitrogen atoms were developed and confirmed (denoted as Ni-PxNy, x = 1, 2 and y = 3, 2). In CO2 reduction reaction (CO2RR), the CO current density on Ni-PxNy was significantly higher than that of Ni-N4 catalyst without phosphorus modification. Besides, Ni-P1N3 performed the highest CO Faradaic efficiency (FECO) of 85.0%–98.0% over a wide potential range of −0.65 to −0.95 V (vs. the reversible hydrogen electrode (RHE)). Experimental and theoretical results revealed that the asymmetric Ni-P1N3 site was beneficial to CO2 intermediate adsorption/desorption, thereby accelerating the reaction kinetics and boosting CO2RR activity. This work provides an effective method for preparing well-defined dual-coordinated SSCs to improve catalytic performance, targetting to CO2RR applications. [Figure not available: see fulltext.]

KW - CO reduction reaction

KW - asymmetric coordination

KW - atomic interface

KW - nickel single-site catalysts

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DO - 10.1007/s12274-022-4969-z

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ER -

Rational design of asymmetric atomic Ni-P₁N₃ active sites for promoting electrochemical CO₂ reduction

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