A Superlattice Imprinting Method to Construct High Ni Single Atoms Inside Ordered Mesoporous Carbon for Efficient Electrocatalysis

Yangyang Ding; Yanxi Hu; Junjun Ge; Jie Guan; Guangtao Wang; Xintian Wang; Yujing Jiang; Jason Chun-Ho Lam; Jiaju Fu; Yuehe Lin; Wenlei Zhu; Yuanyuan Wang

doi:10.31635/ccschem.025.202505938

A Superlattice Imprinting Method to Construct High Ni Single Atoms Inside Ordered Mesoporous Carbon for Efficient Electrocatalysis

Yangyang Ding, Yanxi Hu, Junjun Ge, Jie Guan, Guangtao Wang, Xintian Wang, Yujing Jiang, Jason Chun-Ho Lam, Jiaju Fu, Yuehe Lin^*, Wenlei Zhu^*, Yuanyuan Wang^*

^*Corresponding author for this work

School of Energy and Environment

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

Abstract

Precise design of porous electrocatalysts remains a major challenge for efficient energy conversion. Here, guided by finite element simulations (FES), we have revealed that ordered mesoporous frameworks stabilized gas-liquid-solid interfaces by promoting uniform gas distribution and nanoscale liquid films on hydrophilic surfaces, enhancing mass transfer kinetics. Based on these insights, we developed a superlattice (SL) imprinting method to construct robust three-dimensional (3D) ordered mesoporous carbon (OMC) frameworks embedded with atomically dispersed Ni single atoms. This method integrated confined oxidation for thermal stabilization, ligand-carbonization to preserve SL-derived porosity, acid etching to improve hydrophilicity, high-temperature graphitization for conductivity, and in situ heteroatom doping to optimize Ni coordination. The resulting Ni-N₂S₂ and Ni-N₃P catalysts exhibited excellent electrocatalytic activity, achieving overpotentials of 239 mV [oxygen evolution reaction (OER): 20 mA cm^-2] and 90 mV [hydrogen evolution reaction (HER): 10 mA cm^-2], respectively. A Ni-N₂S₂⁽⁺⁾//Ni-N₃P^(-) electrolyzer delivered stable overall water splitting for over 100 h. This work introduces a simulation-guided framework for tailoring triple-phase equilibria and a confined-oxidation pathway to engineer highly active and durable single-atom electrocatalysts. © 2025 Chinese Chemical Society.

Original language	English
Number of pages	14
Journal	CCS Chemistry
Online published	10 Sept 2025
DOIs	https://doi.org/10.31635/ccschem.025.202505938
Publication status	Online published - 10 Sept 2025

Funding

This work was supported by the National Natural Science Foundation of China (grant nos. 22171132 and 52472165), the Program for Innovative Talents and Entrepreneurs in Jiangsu, China (grant nos. 020513006012 and 020513006014), and the Zijin Scholars Foundation, China (grant no. 0205181022). W.Z. would like to acknowledge the support from National Natural Science Foundation of China (grant no. 22176086), the Fundamental Research Funds for the Central Universities, China (grant nos. 021114380222 and 021114380214), Research Funds for Jiangsu Distinguished Professor, Carbon Peaking and Carbon Neutrality Technological Innovation Foundation of Jiangsu Province (grant no. BE2022861), State Key Laboratory of Analytical Chemistry for Life Science, China (grant no. SKLACLS2503). Y.J. would like to acknowledge the support from the Fundamental Research Funds for the Central Universities-Cemac “GeoX” Interdisciplinary Program and Frontiers Science Center for Critical Earth Material Cycling of Nanjing University, China (grant nos. 2024QNXZ07 and 021114380217). Y.H. would like to acknowledge the support from “GeoX” Interdisciplinary Project of Frontiers Science Center for Critical Earth Material Cycling (grant nos. 20250310 and 021114380235) and College Students’ Innovative Entrepreneurial Training Plan Program, China (grant no. S202510248242).

Research Keywords

single atom catalysts
triple-phase equilibria
ordered mesoporous carbon
finite element simulations
superlattice imprinting

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@article{5168f168705941fc898d6b739da53687,

title = "A Superlattice Imprinting Method to Construct High Ni Single Atoms Inside Ordered Mesoporous Carbon for Efficient Electrocatalysis",

abstract = "Precise design of porous electrocatalysts remains a major challenge for efficient energy conversion. Here, guided by finite element simulations (FES), we have revealed that ordered mesoporous frameworks stabilized gas-liquid-solid interfaces by promoting uniform gas distribution and nanoscale liquid films on hydrophilic surfaces, enhancing mass transfer kinetics. Based on these insights, we developed a superlattice (SL) imprinting method to construct robust three-dimensional (3D) ordered mesoporous carbon (OMC) frameworks embedded with atomically dispersed Ni single atoms. This method integrated confined oxidation for thermal stabilization, ligand-carbonization to preserve SL-derived porosity, acid etching to improve hydrophilicity, high-temperature graphitization for conductivity, and in situ heteroatom doping to optimize Ni coordination. The resulting Ni-N2S2 and Ni-N3P catalysts exhibited excellent electrocatalytic activity, achieving overpotentials of 239 mV [oxygen evolution reaction (OER): 20 mA cm-2] and 90 mV [hydrogen evolution reaction (HER): 10 mA cm-2], respectively. A Ni-N2S2(+)//Ni-N3P(-) electrolyzer delivered stable overall water splitting for over 100 h. This work introduces a simulation-guided framework for tailoring triple-phase equilibria and a confined-oxidation pathway to engineer highly active and durable single-atom electrocatalysts. {\textcopyright} 2025 Chinese Chemical Society.",

keywords = "single atom catalysts, triple-phase equilibria, ordered mesoporous carbon, finite element simulations, superlattice imprinting",

author = "Yangyang Ding and Yanxi Hu and Junjun Ge and Jie Guan and Guangtao Wang and Xintian Wang and Yujing Jiang and Lam, {Jason Chun-Ho} and Jiaju Fu and Yuehe Lin and Wenlei Zhu and Yuanyuan Wang",

year = "2025",

month = sep,

day = "10",

doi = "10.31635/ccschem.025.202505938",

language = "English",

journal = "CCS Chemistry",

issn = "2096-5745",

publisher = "Chinese Chemical Society",

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TY - JOUR

T1 - A Superlattice Imprinting Method to Construct High Ni Single Atoms Inside Ordered Mesoporous Carbon for Efficient Electrocatalysis

AU - Ding, Yangyang

AU - Hu, Yanxi

AU - Ge, Junjun

AU - Guan, Jie

AU - Wang, Guangtao

AU - Wang, Xintian

AU - Jiang, Yujing

AU - Lam, Jason Chun-Ho

AU - Fu, Jiaju

AU - Lin, Yuehe

AU - Zhu, Wenlei

AU - Wang, Yuanyuan

PY - 2025/9/10

Y1 - 2025/9/10

N2 - Precise design of porous electrocatalysts remains a major challenge for efficient energy conversion. Here, guided by finite element simulations (FES), we have revealed that ordered mesoporous frameworks stabilized gas-liquid-solid interfaces by promoting uniform gas distribution and nanoscale liquid films on hydrophilic surfaces, enhancing mass transfer kinetics. Based on these insights, we developed a superlattice (SL) imprinting method to construct robust three-dimensional (3D) ordered mesoporous carbon (OMC) frameworks embedded with atomically dispersed Ni single atoms. This method integrated confined oxidation for thermal stabilization, ligand-carbonization to preserve SL-derived porosity, acid etching to improve hydrophilicity, high-temperature graphitization for conductivity, and in situ heteroatom doping to optimize Ni coordination. The resulting Ni-N2S2 and Ni-N3P catalysts exhibited excellent electrocatalytic activity, achieving overpotentials of 239 mV [oxygen evolution reaction (OER): 20 mA cm-2] and 90 mV [hydrogen evolution reaction (HER): 10 mA cm-2], respectively. A Ni-N2S2(+)//Ni-N3P(-) electrolyzer delivered stable overall water splitting for over 100 h. This work introduces a simulation-guided framework for tailoring triple-phase equilibria and a confined-oxidation pathway to engineer highly active and durable single-atom electrocatalysts. © 2025 Chinese Chemical Society.

AB - Precise design of porous electrocatalysts remains a major challenge for efficient energy conversion. Here, guided by finite element simulations (FES), we have revealed that ordered mesoporous frameworks stabilized gas-liquid-solid interfaces by promoting uniform gas distribution and nanoscale liquid films on hydrophilic surfaces, enhancing mass transfer kinetics. Based on these insights, we developed a superlattice (SL) imprinting method to construct robust three-dimensional (3D) ordered mesoporous carbon (OMC) frameworks embedded with atomically dispersed Ni single atoms. This method integrated confined oxidation for thermal stabilization, ligand-carbonization to preserve SL-derived porosity, acid etching to improve hydrophilicity, high-temperature graphitization for conductivity, and in situ heteroatom doping to optimize Ni coordination. The resulting Ni-N2S2 and Ni-N3P catalysts exhibited excellent electrocatalytic activity, achieving overpotentials of 239 mV [oxygen evolution reaction (OER): 20 mA cm-2] and 90 mV [hydrogen evolution reaction (HER): 10 mA cm-2], respectively. A Ni-N2S2(+)//Ni-N3P(-) electrolyzer delivered stable overall water splitting for over 100 h. This work introduces a simulation-guided framework for tailoring triple-phase equilibria and a confined-oxidation pathway to engineer highly active and durable single-atom electrocatalysts. © 2025 Chinese Chemical Society.

KW - single atom catalysts

KW - triple-phase equilibria

KW - ordered mesoporous carbon

KW - finite element simulations

KW - superlattice imprinting

UR - https://www.webofscience.com/wos/woscc/full-record/WOS:001568334900001

U2 - 10.31635/ccschem.025.202505938

DO - 10.31635/ccschem.025.202505938

M3 - RGC 21 - Publication in refereed journal

SN - 2096-5745

JO - CCS Chemistry

JF - CCS Chemistry

ER -

A Superlattice Imprinting Method to Construct High Ni Single Atoms Inside Ordered Mesoporous Carbon for Efficient Electrocatalysis

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