Recent advances in nickel‐based catalysts in eCO<sub>2</sub>RR for carbon neutrality

Peng, Weikang; Li, Fengfeng; Kong, Shuyi; Guo, Chenxi; Wu, Haotian; Wang, Jiacheng; Shen, Yi; Meng, Xianguang; Zhang, Mingxi

doi:10.1002/cey2.498

Carbon Energy

2024

DOI: 10.1002/cey2.498

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Recent advances in nickel‐based catalysts in eCO₂RR for carbon neutrality

Weikang Peng,

Fengfeng Li,

Shuyi Kong

et al.

Abstract: The excessive use of nonrenewable energy has brought about serious greenhouse effect. Converting CO2 into high‐value‐added chemicals is undoubtedly the best choice to solve energy problems. Due to the excellent cost‐effectiveness and dramatic catalytic performance, nickel‐based catalysts have been considered as the most promising candidates for the electrocatalytic CO2 reduction reaction (eCO2RR). In this work, the electrocatalytic reduction mechanism of CO2 over Ni‐based materials is reviewed. The strategies … Show more

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Cited by 7 publications

References 183 publications

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The Reconstruction of Bi₂Te₄O₁₁ Nanorods for Efficient and pH‐universal Electrochemical CO₂ Reduction

Chen,

Mao,

Wang

et al. 2024

Angewandte Chemie

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The practical application of electrochemical CO2 reduction reaction (CO2RR) is hindered by the competing CO production, hydrogen evolution reaction (HER), and the lack of pH‐universal catalysts. Here, Te‐modified Bi nanorods (Te‐Bi NRs) were synthesized through in situ reconstruction of Bi2Te4O11 NRs under the CO2RR condition. Our study illustrates that the complex reconstruction process of Bi2Te4O11 NRs during CO2RR could be decoupled into three distinct steps, i.e., the destruction of Bi2Te4O11, the formation of Te/Bi phases, and the dissolution of Te. The thus‐obtained Te‐Bi NRs exhibit remarkably high performance in CO2RR towards formate production, showing high activity, selectivity, and stability across all pH conditions (acidic, neutral, and alkaline). In a flow cell reactor under neutral, alkaline, or acidic conditions, the catalysts achieved HCOOH Faradaic efficiencies of up to 94.3%, 96.4%, and 91.0%, respectively, at a high current density of 300 mA cm‐2. DFT calculations, along with operando spectral measurements, reveal that Te manipulates the Bi sites to an electron‐deficient state, enhancing the adsorption strength of the *OCHO intermediate, and significantly suppressing the competing HER and CO production. This study highlights the substantial influence of catalyst reconstruction under operational conditions and offers insights into designing highly active and stable electrocatalysts towards CO2RR.

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The Reconstruction of Bi₂Te₄O₁₁ Nanorods for Efficient and pH‐universal Electrochemical CO₂ Reduction

Chen,

Mao,

Wang

et al. 2024

Angewandte Chemie

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Regulating the Critical Intermediates of Dual‐Atom Catalysts for CO₂Electroreduction

Zhang,

Zhou,

et al. 2024

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Electrocatalysis is a very attractive way to achieve a sustainable carbon cycle by converting CO2 into organic fuels and feedstocks. Therefore, it is crucial to design advanced electrocatalysts by understanding the reaction mechanism of electrochemical CO2 reduction reaction (eCO2RR) with multiple electron transfers. Among electrocatalysts, dual‐atom catalysts (DACs) are promising candidates due to their distinct electronic structures and extremely high atomic utilization efficiency. Herein, the eCO2RR mechanism and the identification of intermediates using advanced characterization techniques, with a particular focus on regulating the critical intermediates are systematically summarized. Further, the insightful understanding of the functionality of DACs originates from the variable metrics of electronic structures including orbital structure, charge distribution, and electron spin state, which influences the active sites and critical intermediates in eCO2RR processes. Based on the intrinsic relationship between variable metrics and critical intermediates, the optimized strategies of DACs are summarized containing the participation of synergistic atoms, engineering of the atomic coordination environment, regulation of the diversity of central metal atoms, and modulation of metal‐support interaction. Finally, the challenges and future opportunities of atomically dispersed catalysts for eCO2RR processes are discussed.

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Boron‐Doped Ti₃C₂T_x MXene for Effective and Durable High‐Current‐Density Ammonia Synthesis

Luo,

Wu,

et al. 2024

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Ammonia (NH3) synthesis via the nitrate reduction reaction (NO3RR) offers a competitive strategy for nitrogen cycling and carbon neutrality; however, this is hindered by the poor NO3RR performance under high current density. Herein, it is shown that boron‐doped Ti3C2Tx MXene nanosheets can highly efficiently catalyze the conversion of NO3RR‐to‐NH3 at ambient conditions, showing a maximal NH3 Faradic efficiency of 91% with a peak yield rate of 26.2 mgh−1 mgcat.−1, and robust durability over ten consecutive cycles, all of them are comparable to the best‐reported results and exceed those of pristine Ti3C2Tx MXene. More importantly, when tested in a flow cell, the designed catalyst delivers a current density of ‒1000 mA cm−2 at a low potential of ‒1.18 V versus the reversible hydrogen electrode and maintains a high NH3 selectivity over a wide current density range. Besides, a Zn–nitrate battery with the catalyst as the cathode is assembled, which achieves a power density of 5.24 mW cm−2 and a yield rate of 1.15 mgh−1 mgcat.−1. Theoretical simulations further demonstrate that the boron dopants can optimize the adsorption and activation of NO3RR intermediates, and reduce the potential‐determining step barrier, thus leading to an enhanced NH3 selectivity.

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Recent advances in nickel‐based catalysts in eCO₂RR for carbon neutrality

Cited by 7 publications

References 183 publications

The Reconstruction of Bi₂Te₄O₁₁ Nanorods for Efficient and pH‐universal Electrochemical CO₂ Reduction

The Reconstruction of Bi₂Te₄O₁₁ Nanorods for Efficient and pH‐universal Electrochemical CO₂ Reduction

Regulating the Critical Intermediates of Dual‐Atom Catalysts for CO₂Electroreduction

Boron‐Doped Ti₃C₂T_x MXene for Effective and Durable High‐Current‐Density Ammonia Synthesis

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Recent advances in nickel‐based catalysts in eCO2RR for carbon neutrality

Cited by 7 publications

References 183 publications

The Reconstruction of Bi2Te4O11 Nanorods for Efficient and pH‐universal Electrochemical CO2 Reduction

The Reconstruction of Bi2Te4O11 Nanorods for Efficient and pH‐universal Electrochemical CO2 Reduction

Regulating the Critical Intermediates of Dual‐Atom Catalysts for CO2Electroreduction

Boron‐Doped Ti3C2Tx MXene for Effective and Durable High‐Current‐Density Ammonia Synthesis

Contact Info

Product

Resources

About

Recent advances in nickel‐based catalysts in eCO₂RR for carbon neutrality

The Reconstruction of Bi₂Te₄O₁₁ Nanorods for Efficient and pH‐universal Electrochemical CO₂ Reduction

The Reconstruction of Bi₂Te₄O₁₁ Nanorods for Efficient and pH‐universal Electrochemical CO₂ Reduction

Regulating the Critical Intermediates of Dual‐Atom Catalysts for CO₂Electroreduction

Boron‐Doped Ti₃C₂T_x MXene for Effective and Durable High‐Current‐Density Ammonia Synthesis