Boosting oxygen reduction performances in Pd-based metallenes by co-confining interstitial H and p-block single atoms

Yu Qiu; Mingzi Sun; Jiandong Wu; Chunxiao Chai; Shengwei Wang; Hong Huang; Xiao Zhao; Dongxu Jiao; Shan Xu; Dewen Wang; Xin Ge; Wei Zhang; Weitao Zheng; Yujiang Song; Jinchang Fan; Bolong Huang; Xiaoqiang Cui

doi:10.1038/s41467-025-60400-5

Boosting oxygen reduction performances in Pd-based metallenes by co-confining interstitial H and p-block single atoms

Yu Qiu (Co-first Author)
, Mingzi Sun (Co-first Author)
, Jiandong Wu
, Chunxiao Chai
, Shengwei Wang
, Hong Huang
, Xiao Zhao
, Dongxu Jiao
, Shan Xu
, Dewen Wang
, Xin Ge
, Wei Zhang
, Weitao Zheng
, Yujiang Song
, Jinchang Fan^*
, Bolong Huang^*
, Xiaoqiang Cui^*

^*Corresponding author for this work

Department of Chemistry

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

32 Citations (Scopus)

95 Downloads (CityUHK Scholars)

Abstract

The efficiency of the oxygen reduction reaction (ORR) is limited by the scaling relationship in the conventional oxygen associative pathway. To break such limitations, we present an approach to effectively activate the oxygen dissociative pathway through co-confining single p-block (In, Sn, Pb) atoms and interstitial H atoms within Pd metallenes, leading to good ORR performance. PdPbH_x metallenes exhibit a high mass activity of 1.36 A mg⁻¹at 0.95 V (vs. RHE), which is 46.9 times higher than that of the benchmark Pt/C. The minimal performance decay after 50,000 potential cycles confirms a good stability. In situ vibrational spectroscopy investigations and theoretical calculations highlight that interstitial H atoms facilitate the direct dissociation of O₂ while single Pb atoms enhance O₂ adsorption strength. The electroactive PdPbHx metallenes is attributed to the up-shifted Pd-4d orbitals induced by H and Pb atoms. This research supplies critical inspiration for developing highly efficient ORR electrocatalysts.

© The Author(s) 2025

Original language	English
Number of pages	382
Journal	Nature Communications
Volume	16
Online published	6 Jun 2025
DOIs	https://doi.org/10.1038/s41467-025-60400-5
Publication status	Published - 2025

Funding

J. Fan and X. Cui acknowledged the support of the National Natural Science Foundation of China (12034002 (X.C.), 22279044 (X.C.), and 22402064 (J.F.)). B.H. acknowledged the support of the National Key R&D Program of China (2021YFA1501101), Research Grant Council of Hong Kong (15304023, 15304724, C1003-23Y), National Natural Science Foundation of China/Research Grant Council of Hong Kong Joint Research Scheme (N_PolyU502/21), the National Natural Science Foundation of China/Research Grants Council of Hong Kong Collaborative Research Scheme (CRS_PolyU504/22), the Shenzhen Fundamental Research Scheme-General Program (JCYJ20220531090807017), and the Natural Science Foundation of Guangdong Province (2023A1515012219).

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title = "Boosting oxygen reduction performances in Pd-based metallenes by co-confining interstitial H and p-block single atoms",

abstract = "The efficiency of the oxygen reduction reaction (ORR) is limited by the scaling relationship in the conventional oxygen associative pathway. To break such limitations, we present an approach to effectively activate the oxygen dissociative pathway through co-confining single p-block (In, Sn, Pb) atoms and interstitial H atoms within Pd metallenes, leading to good ORR performance. PdPbHx metallenes exhibit a high mass activity of 1.36 A mg−1 at 0.95 V (vs. RHE), which is 46.9 times higher than that of the benchmark Pt/C. The minimal performance decay after 50,000 potential cycles confirms a good stability. In situ vibrational spectroscopy investigations and theoretical calculations highlight that interstitial H atoms facilitate the direct dissociation of O2 while single Pb atoms enhance O2 adsorption strength. The electroactive PdPbHx metallenes is attributed to the up-shifted Pd-4d orbitals induced by H and Pb atoms. This research supplies critical inspiration for developing highly efficient ORR electrocatalysts. {\textcopyright} The Author(s) 2025",

author = "Yu Qiu and Mingzi Sun and Jiandong Wu and Chunxiao Chai and Shengwei Wang and Hong Huang and Xiao Zhao and Dongxu Jiao and Shan Xu and Dewen Wang and Xin Ge and Wei Zhang and Weitao Zheng and Yujiang Song and Jinchang Fan and Bolong Huang and Xiaoqiang Cui",

year = "2025",

doi = "10.1038/s41467-025-60400-5",

language = "English",

volume = "16",

journal = "Nature Communications",

issn = "2041-1723",

publisher = "Springer Nature",

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TY - JOUR

T1 - Boosting oxygen reduction performances in Pd-based metallenes by co-confining interstitial H and p-block single atoms

AU - Qiu, Yu

AU - Sun, Mingzi

AU - Wu, Jiandong

AU - Chai, Chunxiao

AU - Wang, Shengwei

AU - Huang, Hong

AU - Zhao, Xiao

AU - Jiao, Dongxu

AU - Xu, Shan

AU - Wang, Dewen

AU - Ge, Xin

AU - Zhang, Wei

AU - Zheng, Weitao

AU - Song, Yujiang

AU - Fan, Jinchang

AU - Huang, Bolong

AU - Cui, Xiaoqiang

PY - 2025

Y1 - 2025

N2 - The efficiency of the oxygen reduction reaction (ORR) is limited by the scaling relationship in the conventional oxygen associative pathway. To break such limitations, we present an approach to effectively activate the oxygen dissociative pathway through co-confining single p-block (In, Sn, Pb) atoms and interstitial H atoms within Pd metallenes, leading to good ORR performance. PdPbHx metallenes exhibit a high mass activity of 1.36 A mg−1 at 0.95 V (vs. RHE), which is 46.9 times higher than that of the benchmark Pt/C. The minimal performance decay after 50,000 potential cycles confirms a good stability. In situ vibrational spectroscopy investigations and theoretical calculations highlight that interstitial H atoms facilitate the direct dissociation of O2 while single Pb atoms enhance O2 adsorption strength. The electroactive PdPbHx metallenes is attributed to the up-shifted Pd-4d orbitals induced by H and Pb atoms. This research supplies critical inspiration for developing highly efficient ORR electrocatalysts. © The Author(s) 2025

AB - The efficiency of the oxygen reduction reaction (ORR) is limited by the scaling relationship in the conventional oxygen associative pathway. To break such limitations, we present an approach to effectively activate the oxygen dissociative pathway through co-confining single p-block (In, Sn, Pb) atoms and interstitial H atoms within Pd metallenes, leading to good ORR performance. PdPbHx metallenes exhibit a high mass activity of 1.36 A mg−1 at 0.95 V (vs. RHE), which is 46.9 times higher than that of the benchmark Pt/C. The minimal performance decay after 50,000 potential cycles confirms a good stability. In situ vibrational spectroscopy investigations and theoretical calculations highlight that interstitial H atoms facilitate the direct dissociation of O2 while single Pb atoms enhance O2 adsorption strength. The electroactive PdPbHx metallenes is attributed to the up-shifted Pd-4d orbitals induced by H and Pb atoms. This research supplies critical inspiration for developing highly efficient ORR electrocatalysts. © The Author(s) 2025

UR - https://www.webofscience.com/wos/woscc/full-record/WOS:001504287800011

U2 - 10.1038/s41467-025-60400-5

DO - 10.1038/s41467-025-60400-5

M3 - RGC 21 - Publication in refereed journal

C2 - 40481022

SN - 2041-1723

VL - 16

JO - Nature Communications

JF - Nature Communications

ER -

Boosting oxygen reduction performances in Pd-based metallenes by co-confining interstitial H and p-block single atoms

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GRF: Flexible Atomic Catalysts for Full Spectrum Photocatalytic Production of Syngas via Machine Learning Acceleration

YCRG: Electrochemical Lithium Intercalation & Exfoliation for Mass Production of 2D Transition Metal Dichalcogenides and their Application for Water Purification

GRF: Developing Advanced Carbon-Skeleton Supported Atomic Catalysts for C2 Products of CO2 Reduction Reaction

Cite this

Boosting oxygen reduction performances in Pd-based metallenes by co-confining interstitial H and p-block single atoms

Abstract

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Publisher's Copyright Statement

RGC Funding Information

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Projects

GRF: Flexible Atomic Catalysts for Full Spectrum Photocatalytic Production of Syngas via Machine Learning Acceleration

YCRG: Electrochemical Lithium Intercalation & Exfoliation for Mass Production of 2D Transition Metal Dichalcogenides and their Application for Water Purification

GRF: Developing Advanced Carbon-Skeleton Supported Atomic Catalysts for C2 Products of CO2 Reduction Reaction

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