Screening MXene-based single-atom catalysts for selective nitrate-to-ammonia electroreduction

Wang, Mengting; Hu, Tao; Wang, Changhong; Du, Feng; Yang, Hongbin; Sun, Wei; Guo, Chunxian; Li, Chang Ming

doi:10.1007/s40843-022-2406-5

Cited by 15 publications

(1 citation statement)

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“…In recent years, numerous catalysts have been designed for application in Ph–NH 2 production, mainly including noble metal catalysts, non-noble metal catalysts, and metal-free carbon catalysts. , Among them, noble metal catalysts such as palladium (Pb), platinum (Pt), and ruthenium (Ru) have shown excellent activities in the catalytic hydrogenation of nitroaromatics. , However, due to high costs and low natural abundances, noble metal catalysts cannot meet the increasing demands. Therefore, the exploration of economical, efficient, and environment-friendly catalysts for aniline synthesis is the focus of catalytic technology development at present. − …”

Section: Introductionmentioning

confidence: 99%

Insights into the Mechanism of Nitrobenzene Reduction to Aniline by Phosphomolybdic Acid Supported TM₁ Single-Atom Catalysts

Zhao,

Wang,

Yan

et al. 2024

Inorg. Chem.

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Catalytic hydrogenation of nitrobenzene (Ph–NO2) to aniline (Ph–NH2) is a model reaction in the field of catalysis, in which the development of efficient catalysts remains a great challenge due to the lack of strategies to solve activity and selectivity problems. In this work, the mechanism of Ph–NO2 hydrogenation over Pt1 supported on phosphomolybdic acid (α-PMA) was proposed by density functional theory (DFT) calculations. The results show that the dissociation of the first and second N–O bonds is triggered by single H-induced and double H-induced mechanisms, respectively. The limiting potential of the reaction process is −0.19 V, which is the smallest potential in the field of Ph–NO2 reduction reaction to date. In the whole reaction process, the catalytic active site is the Pt atom, and polyoxometalate plays the role of an electronic sponge in the reaction. Additionally, based on experimentally confirmed Pt1/Na3PMA, the reduction capacity of Pd1/Na3PMA toward Ph–NO2 was predicted by DFT calculation. The distinctive adsorption patterns of Ph–NO2 on Pt1/Na3PMA and Pd1/Na3PMA were elucidated using the DOS diagram and fragment molecular orbital analysis. We anticipate that our theoretical calculations can provide novel perspectives for experimental researchers.

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Section: Introductionmentioning

confidence: 99%

Insights into the Mechanism of Nitrobenzene Reduction to Aniline by Phosphomolybdic Acid Supported TM₁ Single-Atom Catalysts

Zhao,

Wang,

Yan

et al. 2024

Inorg. Chem.

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Electrochemical Nitrate Reduction to Ammonia – Recent Progress

Niu,

Yang,

Qian

et al. 2023

ChemElectroChem

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The presence of nitrate in industrial, domestic and agricultural wastewater has a detrimental impact on both ecosystem and human health, as remediation and purification efforts are slow, challenging and difficult, given the high solubility and stability of this pollutant. Taking nitrate into high value‐added ammonia by electrochemical reduction can overcome high pollution and energy consumption limit of Haber‐Bosch process with long‐term significance of environmental protection and energy saving. This review summarized the research progress on the electrocatalytic reduction of nitrate to ammonia, with a focus on the reaction mechanisms, influencing factors, product detection methods, performance evaluation methods and the research status of electrocatalysts up to now. The review reported the latest strategies employed to design efficient electrocatalysts, such as pore structure regulation, alloying, heterostructure construction, defect and interface engineering, crystal surface regulation and microenvironment modulation of single‐atom catalysts. It highlights critical factors that determin the performance in terms of nitrate adsorption, exposed active sites, mass transfer rate, intermediates barrier and side reactions, as well as the stability of electrocatalysts and recovery of ammonia. In addition, the future direction of technology for electrocatalytic reduction of nitrate to ammonia has also been proposed.

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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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Screening MXene-based single-atom catalysts for selective nitrate-to-ammonia electroreduction

Cited by 15 publications

References 53 publications

Insights into the Mechanism of Nitrobenzene Reduction to Aniline by Phosphomolybdic Acid Supported TM₁ Single-Atom Catalysts

Insights into the Mechanism of Nitrobenzene Reduction to Aniline by Phosphomolybdic Acid Supported TM₁ Single-Atom Catalysts

Electrochemical Nitrate Reduction to Ammonia – Recent Progress

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

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Screening MXene-based single-atom catalysts for selective nitrate-to-ammonia electroreduction

Cited by 15 publications

References 53 publications

Insights into the Mechanism of Nitrobenzene Reduction to Aniline by Phosphomolybdic Acid Supported TM1 Single-Atom Catalysts

Insights into the Mechanism of Nitrobenzene Reduction to Aniline by Phosphomolybdic Acid Supported TM1 Single-Atom Catalysts

Electrochemical Nitrate Reduction to Ammonia – Recent Progress

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

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Product

Resources

About

Insights into the Mechanism of Nitrobenzene Reduction to Aniline by Phosphomolybdic Acid Supported TM₁ Single-Atom Catalysts

Insights into the Mechanism of Nitrobenzene Reduction to Aniline by Phosphomolybdic Acid Supported TM₁ Single-Atom Catalysts

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