Active hydrogen-controlled CO&lt;sub&gt;2&lt;/sub&gt;/N&lt;sub&gt;2&lt;/sub&gt;/NO&lt;sub&gt;x&lt;/sub&gt; electroreduction:From mechanism understanding to catalyst design

Liu, Hanle; Jia, Shunhan; Wu, Limin; He, Lei; Sun, Xiaofu; Han, Buxing

doi:10.59717/j.xinn-mater.2024.100058

TIMS

2024

DOI: 10.59717/j.xinn-mater.2024.100058

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Active hydrogen-controlled CO2/N2/NOx electroreduction:From mechanism understanding to catalyst design

Hanle Liu,

Shunhan Jia,

Limin Wu

et al.

Abstract: The development of renewable-energy-powered electrocatalysis meets the need for the sustainable society. With water as the proton source, it enables efficient production of chemicals and fuels from renewable resources like CO2, N2, and NOx under ambient conditions. Hydrogen generated via water dissociation is a crucial participant in transforming reactants into desired products, but it also serves as a direct source of undesired reac… Show more

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Cited by 3 publications

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The Loss of Interfacial Water-Adsorbate Hydrogen Bond Connectivity Position Surface-Active Hydrogen as a Crucial Intermediate to Enhance Nitrate Reduction Reaction

Zheng,

Yang,

Shi

et al. 2024

J. Am. Chem. Soc.

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The electrochemical nitrate reduction reaction (NO 3 RR) offers a promising solution for remediating nitrate-polluted wastewater while enabling the sustainable production of ammonia. The control strategy of surface-active hydrogen (*H) is extensively employed to enhance the kinetics of the NO 3 RR, but atomic understanding lags far behind the experimental observations. Here, we decipher the cation-water-adsorbate interactions in regulating the NO 3 RR kinetics at the Cu (111) electrode/electrolyte interface using AIMD simulations with a slow-growth approach. We demonstrate that the key oxygen-containing intermediates of the NO 3 RR (e.g., *NO, *NO 2 , and *NO 3 ) will stably coordinate with the cations, impeding their integration with the hydrogen bond network and further their hydrogenation by interfacial water molecules due to steric hindrance. The *H can migrate across the interface with a low energy barrier, and its hydrogenation barrier with oxygen-containing species remains unaffected by cations, offering a potent supplement to the hydrogenation process, playing the predominant factor by which the *H facilitates NO 3 RR reaction kinetic. This study provides valuable insights for understanding the reaction mechanism of NO 3 RR by fully considering the cation−water−adsorbate interactions, which can aid in the further development of the electrolyte and electrocatalysts for efficient NO 3 RR.

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The Loss of Interfacial Water-Adsorbate Hydrogen Bond Connectivity Position Surface-Active Hydrogen as a Crucial Intermediate to Enhance Nitrate Reduction Reaction

Zheng,

Yang,

Shi

et al. 2024

J. Am. Chem. Soc.

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Essential features of weak current for excellent enhancement of NOx reduction over monoatomic V-based catalyst

Zheng,

Liu,

Zhang

et al. 2024

Nat Commun

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Human society is facing increasingly serious problems of environmental pollution and energy shortage, and up to now, achieving high NH 3 -SCR activity at ultra-low temperatures (<150 °C) remains challenging for the V-based catalysts with V content below 2%. In this study, the monoatomic V-based catalyst under the weak current-assisted strategy can completely convert NO x into N 2 at ultra-low temperature with V content of 1.36%, which shows the preeminent turnover frequencies (TOF 145 °C = 1.97×10 −3 s −1 ). The improvement of catalytic performance is mainly attributed to the enhancement catalysis of weak current (ECWC) rather than electric field, which significantly reduce the energy consumption of the catalytic system by more than 90%. The further mechanism research for the ECWC based on a series of weak current-assisted characterization means and DFT calculations confirms that migrated electrons mainly concentrate around the V single atoms and increase the proportion of antibonding orbitals, which make the V-O chemical bond weaker (electron scissors effect) and thus accelerate oxygen circulation. The novel current-assisted catalysis in the present work can potentially apply to other environmental and energy fields.

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Heterogeneous catalysis for the environment

Liu,

Burciaga,

Tang

et al. 2024

TIMS

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Anthropogenic climate and environmental changes increasingly threaten the sustainability of life on Earth, hindering the sustainable development of human societies. These detrimental ecological changes are driven by human activities that have elevated atmospheric levels of greenhouse gases and toxic substances, increased inorganic and organic pollutants in water bodies, and led to the accumulation of solid waste in soils. Over the next two to three decades, the impacts of climate change, water pollution, and soil contamination are expected to intensify, posing increasing risks to human health and global stability. Considering these trends, it is essential to implement robust mitigation and adaptation strategies. This paper analyzes environmental pollution problems from the perspectives of atmospheric, water, and soil contamination. It summarizes current research on heterogeneous catalysis for treating pollutants in gaseous, liquid, and solid phases, with an emphasis on the key challenges of applying these catalytic conversion technologies in cost-effective industrial settings. Finally, strategies for mitigating environmental pollutants via heterogeneous catalysis are discussed from the perspectives of material flow, energy flow, and data flow. This paper aims to offer scientific insights to enhance future research and practice in heterogeneous catalysis for environmental remediation.

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Active hydrogen-controlled CO<sub>2</sub>/N<sub>2</sub>/NO<sub>x</sub> electroreduction:From mechanism understanding to catalyst design

Cited by 3 publications

References 120 publications

The Loss of Interfacial Water-Adsorbate Hydrogen Bond Connectivity Position Surface-Active Hydrogen as a Crucial Intermediate to Enhance Nitrate Reduction Reaction

The Loss of Interfacial Water-Adsorbate Hydrogen Bond Connectivity Position Surface-Active Hydrogen as a Crucial Intermediate to Enhance Nitrate Reduction Reaction

Essential features of weak current for excellent enhancement of NOx reduction over monoatomic V-based catalyst

Heterogeneous catalysis for the environment

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