Single Nb atom modified anatase TiO2(110) for efficient electrocatalytic nitrogen reduction reaction

Yunnan Gao; Yang Yang; Leiduan Hao; Song Hong; Xinyi Tan; Tai Sing Wu; Yun Liang Soo; Alex W. Robertson; Qi Yang; Zhenyu Sun

doi:10.1016/j.checat.2022.06.010

Single Nb atom modified anatase TiO₂(110) for efficient electrocatalytic nitrogen reduction reaction

Yunnan Gao, Yang Yang, Leiduan Hao, Song Hong, Xinyi Tan^*, Tai Sing Wu, Yun Liang Soo, Alex W. Robertson, Qi Yang^*, Zhenyu Sun^*

^*Corresponding author for this work

School of Material Science and Engineering

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

34 Citations (Scopus)

Abstract

We report the theory-guided design of anatase-supported Nb catalysts for electrochemical N₂ reduction reaction (NRR). Theoretical calculations predict that Nb atoms deliver multi-functional enhancement toward the NRR when incorporated in an anatase TiO₂(110) catalyst: (1) decreasing the band gap and inducing electrons to promote the conductivity of TiO₂(110); (2) suppressing the undesired competitive hydrogen evolution reaction; (3) activating the inert Ti sites for N₂ adsorption; (4) enabling fast charge transfer between ∗NNH and the TiO₂(110) surface; and (5) reducing the energy barrier of the potential-determining ∗N₂ → ∗NNH step, further facilitating NH₃ formation. As a result, our Nb-TiO₂(110) catalyst exhibits superior activity and selectivity for the NRR, which affords an NH₃ production rate of about 21.3 μg h⁻¹ mg_cat⁻¹ and NH₃ faradaic efficiency of ∼9.2% at −0.5 V (versus reversible hydrogen electrode). This study provides insights for the rational design of efficient electrocatalysts for the NRR.

Original language	English
Pages (from-to)	2275-2288
Number of pages	14
Journal	Chem Catalysis
Volume	2
Issue number	9
DOIs	https://doi.org/10.1016/j.checat.2022.06.010
Publication status	Published - 15 Sept 2022

Keywords

N reduction reaction
NH
SDG7: Affordable and clean energy
anatase TiO
crystal facet
density functional theory
electrocatalysis
single atom

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title = "Single Nb atom modified anatase TiO2(110) for efficient electrocatalytic nitrogen reduction reaction",

abstract = "We report the theory-guided design of anatase-supported Nb catalysts for electrochemical N2 reduction reaction (NRR). Theoretical calculations predict that Nb atoms deliver multi-functional enhancement toward the NRR when incorporated in an anatase TiO2(110) catalyst: (1) decreasing the band gap and inducing electrons to promote the conductivity of TiO2(110); (2) suppressing the undesired competitive hydrogen evolution reaction; (3) activating the inert Ti sites for N2 adsorption; (4) enabling fast charge transfer between ∗NNH and the TiO2(110) surface; and (5) reducing the energy barrier of the potential-determining ∗N2 → ∗NNH step, further facilitating NH3 formation. As a result, our Nb-TiO2(110) catalyst exhibits superior activity and selectivity for the NRR, which affords an NH3 production rate of about 21.3 μg h−1 mgcat−1 and NH3 faradaic efficiency of ∼9.2% at −0.5 V (versus reversible hydrogen electrode). This study provides insights for the rational design of efficient electrocatalysts for the NRR.",

keywords = "N reduction reaction, NH, SDG7: Affordable and clean energy, anatase TiO, crystal facet, density functional theory, electrocatalysis, single atom",

author = "Yunnan Gao and Yang Yang and Leiduan Hao and Song Hong and Xinyi Tan and Wu, {Tai Sing} and Soo, {Yun Liang} and Robertson, {Alex W.} and Qi Yang and Zhenyu Sun",

note = "Publisher Copyright: {\textcopyright} 2022 Elsevier Inc.",

year = "2022",

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day = "15",

doi = "10.1016/j.checat.2022.06.010",

language = "English",

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T1 - Single Nb atom modified anatase TiO2(110) for efficient electrocatalytic nitrogen reduction reaction

AU - Gao, Yunnan

AU - Yang, Yang

AU - Hao, Leiduan

AU - Hong, Song

AU - Tan, Xinyi

AU - Wu, Tai Sing

AU - Soo, Yun Liang

AU - Robertson, Alex W.

AU - Yang, Qi

AU - Sun, Zhenyu

PY - 2022/9/15

Y1 - 2022/9/15

N2 - We report the theory-guided design of anatase-supported Nb catalysts for electrochemical N2 reduction reaction (NRR). Theoretical calculations predict that Nb atoms deliver multi-functional enhancement toward the NRR when incorporated in an anatase TiO2(110) catalyst: (1) decreasing the band gap and inducing electrons to promote the conductivity of TiO2(110); (2) suppressing the undesired competitive hydrogen evolution reaction; (3) activating the inert Ti sites for N2 adsorption; (4) enabling fast charge transfer between ∗NNH and the TiO2(110) surface; and (5) reducing the energy barrier of the potential-determining ∗N2 → ∗NNH step, further facilitating NH3 formation. As a result, our Nb-TiO2(110) catalyst exhibits superior activity and selectivity for the NRR, which affords an NH3 production rate of about 21.3 μg h−1 mgcat−1 and NH3 faradaic efficiency of ∼9.2% at −0.5 V (versus reversible hydrogen electrode). This study provides insights for the rational design of efficient electrocatalysts for the NRR.

AB - We report the theory-guided design of anatase-supported Nb catalysts for electrochemical N2 reduction reaction (NRR). Theoretical calculations predict that Nb atoms deliver multi-functional enhancement toward the NRR when incorporated in an anatase TiO2(110) catalyst: (1) decreasing the band gap and inducing electrons to promote the conductivity of TiO2(110); (2) suppressing the undesired competitive hydrogen evolution reaction; (3) activating the inert Ti sites for N2 adsorption; (4) enabling fast charge transfer between ∗NNH and the TiO2(110) surface; and (5) reducing the energy barrier of the potential-determining ∗N2 → ∗NNH step, further facilitating NH3 formation. As a result, our Nb-TiO2(110) catalyst exhibits superior activity and selectivity for the NRR, which affords an NH3 production rate of about 21.3 μg h−1 mgcat−1 and NH3 faradaic efficiency of ∼9.2% at −0.5 V (versus reversible hydrogen electrode). This study provides insights for the rational design of efficient electrocatalysts for the NRR.

KW - N reduction reaction

KW - NH

KW - SDG7: Affordable and clean energy

KW - anatase TiO

KW - crystal facet

KW - density functional theory

KW - electrocatalysis

KW - single atom

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JO - Chem Catalysis

JF - Chem Catalysis

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Single Nb atom modified anatase TiO₂(110) for efficient electrocatalytic nitrogen reduction reaction

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