Boosting Low-Temperature CO2 Hydrogenation over Ni-based Catalysts by Tuning Strong Metal-Support Interactions

Runping Ye; Lixuan Ma; Xiaoling Hong; Tomas Ramirez Reina; Wenhao Luo; Liqun Kang; Gang Feng; Rongbin Zhang; Maohong Fan; Riguang Zhang; Jian Liu

doi:10.1002/anie.202317669

Boosting Low-Temperature CO₂ Hydrogenation over Ni-based Catalysts by Tuning Strong Metal-Support Interactions

Angew Chem Int Ed Engl. 2024 Jan 15;63(3):e202317669. doi: 10.1002/anie.202317669. Epub 2023 Dec 8.

Authors

Runping Ye¹, Lixuan Ma², Xiaoling Hong³, Tomas Ramirez Reina⁴, Wenhao Luo⁵, Liqun Kang⁶, Gang Feng¹, Rongbin Zhang¹, Maohong Fan⁷, Riguang Zhang², Jian Liu^{3

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Affiliations

¹ Key Laboratory of Jiangxi Province for Environment and Energy Catalysis, Institute of Applied Chemistry, School of Chemistry and Chemical Engineering, Nanchang University, Nanchang, 330031, P. R. China.
² State Key Laboratory of Clean and Efficient Coal Utilization, College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan, 030024, Shanxi, P. R. China.
³ State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, Liaoning, P. R. China.
⁴ Department of Inorganic Chemistry and Material Sciences Institute of Seville, University of Seville-CSIC, 41092, Seville, Spain.
⁵ College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot, 010021, P. R. China.
⁶ Max Planck Institute for Chemical Energy Conversion, Stiftstraße 34-36, 45470, Mülheim an der Ruhr, Germany.
⁷ College of Engineering and Physical Sciences, and School of Energy Resources, University of Wyoming, Laramie, WY 82071, USA.
⁸ DICP-Surrey Joint Centre for Future Materials, Department of Chemical and Process Engineering, and Advanced Technology Institute, University of Surrey, Guilford, Surrey, GU2 7XH, UK.

PMID: 38032335
DOI: 10.1002/anie.202317669

Abstract

Rational design of low-cost and efficient transition-metal catalysts for low-temperature CO₂ activation is significant and poses great challenges. Herein, a strategy via regulating the local electron density of active sites is developed to boost CO₂ methanation that normally requires >350 °C for commercial Ni catalysts. An optimal Ni/ZrO₂ catalyst affords an excellent low-temperature performance hitherto, with a CO₂ conversion of 84.0 %, CH₄ selectivity of 98.6 % even at 230 °C and GHSV of 12,000 mL g^-1 h^-1 for 106 h, reflecting one of the best CO₂ methanation performance to date on Ni-based catalysts. Combined a series of in situ spectroscopic characterization studies reveal that re-constructing monoclinic-ZrO₂ supported Ni species with abundant oxygen vacancies can facilitate CO₂ activation, owing to the enhanced local electron density of Ni induced by the strong metal-support interactions. These findings might be of great aid for construction of robust catalysts with an enhanced performance for CO₂ emission abatement and beyond.

Keywords: CO2 Methanation; Low-Temperature Activity; Ni-Based Catalysts; Reaction Pathway; Strong Metal-Support Interactions.

Abstract

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