Stable hydroxyl-anchored CuNi nanocatalysts from CuNiMgAl-LDH thermal reduction for efficient photothermal CO2 conversion

Zhijie Wang, Yimian Zhou, Wenkang Ni, Jianfei Li, Xuanyu Yue (), Zizhong Zhang (), Wenxin Dai () and Xianzhi Fu
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Zhijie Wang: Fuzhou University, State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry
Yimian Zhou: Fuzhou University, State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry
Wenkang Ni: Fuzhou University, State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry
Jianfei Li: Fuzhou University, State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry
Xuanyu Yue: Zhejiang University, State Key Laboratory of Biobased Transportation Fuel Technology, College of Biosystems Engineering and Food Science
Zizhong Zhang: Fuzhou University, State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry
Wenxin Dai: Fuzhou University, State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry
Xianzhi Fu: Fuzhou University, State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Cu-based nanocatalysts hold promise for the reverse water–gas shift (RWGS) reaction. However, irreversible sintering of the Cu catalyst for deactivation remains a persistent challenge under thermal or photothermal processes. In this study, we develop an anti-sintering catalyst using CuNiMgAl layered-double-hydroxide (LDH)-derived hydroxyl engineering to anchor ultrafine CuNi nanoparticles, achieving stable photothermal RWGS conversion. For Cu3Ni-MA, the oxyphilic Ni dopants facilitate the formation of hydroxyl-coordinated Cu2+–Ni2+ species during the calcination of LDH-derived materials; meanwhile, the Ni incorporation enhances the plasmonic effect of CuNi nanocatalysts to drive H2 spillover for hydroxyl replenishment under light irradiation, which is diverged from conventional Cu3Ni alloy-based catalysts. This Cu3Ni-MA achieves a CO production rate of 339.8 mmol g−1 h−1 with 98% selectivity, outperforming thermal catalysis by 3.5-fold in RWGS conversion. Notably, the catalyst exhibits robust photothermal CO2 hydrogenation stability, preserving >99% of its original activity and CO selectivity during 30 d of intermittent start–stop cycles and 280-h continuous testing. This study offers alternative perspectives for designing anti-sintering catalysts for photothermal catalytic systems by coupling dynamic hydroxyl regulation with plasmonic activation mechanisms.

Date: 2025
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DOI: 10.1038/s41467-025-65537-x

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