Atomic Distance Engineering in Metal Catalysts to Regulate Catalytic Performance

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(3)

Published: Oct. 2, 2023

Abstract It is very important to understand the structure–performance relationship of metal catalysts by adjusting microstructure at atomic scale. The distance has an essential influence on composition environment active atom, which a key factor for design targeted with desired function. In this review, we discuss and summarize strategies changing from three aspects relate their effects reactivity catalysts. First, regulating bond length between coordination atom one single‐atom site catalytic performance are introduced. lengths affected strain effect support high‐shell doping can evolve during reaction. Next, sites discussed. Due space matching adsorption electron transport, be adjusted shortening distance. addition, arrangement spacing surface atoms nanocatalysts studied. Finally, comprehensive summary outlook given.

Language: Английский

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Free-standing membrane incorporating single-atom catalysts for ultrafast electroreduction of low-concentration nitrate

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(11)

Published: March 6, 2023

The release of wastewaters containing relatively low levels nitrate (NO3-) results in sufficient contamination to induce harmful algal blooms and elevate drinking water NO3- concentrations potentially hazardous levels. In particular, the facile triggering by ultra-low necessitates development efficient methods for destruction. However, promising electrochemical suffer from weak mass transport under reactant concentrations, resulting long treatment times (on order hours) complete this study, we present flow-through electrofiltration via an electrified membrane incorporating nonprecious metal single-atom catalysts reduction activity enhancement selectivity modification, achieving near-complete removal concentration (10 mg-N L-1) with a residence time only few seconds s). By anchoring Cu single atoms supported on N-doped carbon nanotube interwoven framework, fabricate free-standing carbonaceous featuring high conductivity, permeability, flexibility. achieves over 97% N2 86% single-pass electrofiltration, which is significant improvement flow-by operation (30% 7% selectivity). This performance attributed greater adsorption nitric oxide molecular collision frequency coupled balanced supply atomic hydrogen through H2 dissociation during electrofiltration. Overall, our findings provide paradigm applying improve rate purification.

Language: Английский

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Electrocatalytic nitrate reduction to ammonia coupled with organic oxidation

Chem Catalysis, Journal Year: 2023, Volume and Issue: 3(6), P. 100638 - 100638

Published: May 16, 2023

Language: Английский

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Single Atom Environmental Catalysis: Influence of Supports and Coordination Environments

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(50)

Published: Aug. 27, 2023

Abstract Single‐atom catalysts (SACs) are desirable in environmental catalysis due to friendliness, structural stability, and maximum utilization of active metal sites. Extensive research has compared the catalytic performance between SACs with different single‐atom metals. However, their is also highly dependent on supports, which play an important role modulating local coordination environment SACs. Unfortunately, a comprehensive review that systematically discusses relationship supports environment, as well combined effects scare. In this review, three widely investigated applications including advanced oxidation processes (AOPs), mainly Fenton Fenton‐like reactions, nitrate reduction reaction (NO 3 RR) focused. By correlating characterization results, performances, computational environments reactivity examined detail, from origin pathways AOPs NO RR attempted reveal. Finally look forward for potential opportunities challenges on‐demand applications, provided.

Language: Английский

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Metal–support interactions for heterogeneous catalysis: mechanisms, characterization techniques and applications

Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(16), P. 8540 - 8572

Published: Jan. 1, 2023

Metal–support interactions (MSIs) is essential for the understanding of structure–performance relationship and designing in heterogeneous catalysis area. This review mainly summarizes current theoretical experimental research MSIs.

Language: Английский

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Boronization of Nickel Foam for Sustainable Electrochemical Reduction of Nitrate to Ammonia

ACS Energy Letters, Journal Year: 2023, Volume and Issue: 8(9), P. 3843 - 3851

Published: Aug. 22, 2023

Electrochemical reduction of aqueous nitrates has emerged as a sustainable and practical approach in combining water treatment ammonia fertilizer synthesis. However, the development highly integrated catalytic electrodes with consistently high activity from non-noble metals remains challenging issue despite potential to greatly decrease costs promote real-world applications. Here, we report high-performance electrode electron-abundant surfaces obtained direct boronization nickel foam, rendering stable yield rate 19.2 mg h–1 cm–2 Faradaic efficiency 94% for NO3–-to-NH3 conversion. The microprocessing lowers work function initiates local electric field foam by converting acid-stable surface oxides into dyadic nanosheets composed metallic amorphous borates, thus promoting adsorption transformation nitrate anions. Furthermore, spent enables rapid effective regeneration undergoing another round boronization, which ensures long lifetime application our design.

Language: Английский

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Electron-deficient cobalt nanocrystals for promoted nitrate electrocatalytic reduction to synthesize ammonia

Nano Energy, Journal Year: 2023, Volume and Issue: 117, P. 108901 - 108901

Published: Sept. 13, 2023

Language: Английский

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Tailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transfer

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 30, 2024

Abstract The rational design of carbon-supported transition-metal single-atom catalysts requires the precise arrangement heteroatoms within catalysts. However, achieving this is challenging due to collapse structure during pyrolysis. Here, we introduce a topological heteroatom-transfer strategy prevent and accurately control P coordination in As an illustration, have prepared self-assembled helical fibers with encapsulated cavities. Within these cavities, adjustable functional groups can chelate metal ions (N x ···M n+ ···O y ), facilitating preservation pyrolysis based phosphidation. This process allows for transfer from assembly into catalysts, resulting tailoring. Notably, Co–P 2 N –C catalyst exhibits electrocatalytic performance as non-noble alkaline hydrogen evolution, attaining current density 100 mA cm −2 overpotential only 131 mV.

Language: Английский

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Gradient-concentration RuCo electrocatalyst for efficient and stable electroreduction of nitrate into ammonia

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: July 25, 2024

Electrocatalytic nitrate reduction to ammonia holds great promise for developing green technologies electrochemical energy conversion and storage. Considering that real resources often exhibit low concentrations, it is challenging achieve high activity in low-concentration solutions due the competing reaction of hydrogen evolution reaction, let alone considering catalyst lifetime. Herein, we present a performance electrocatalyst based on Co nanosheet structure with gradient dispersion Ru, which yields NH

Language: Английский

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Bioinspired Tandem Electrode for Selective Electrocatalytic Synthesis of Ammonia from Aqueous Nitrate

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(4), P. 2144 - 2152

Published: Jan. 18, 2024

The electrocatalytic nitrate reduction reaction (NO3RR) has recently emerged as a promising technique for readily converting aqueous (NO3–) pollutants into valuable ammonia (NH3). It is vital to thoroughly understand the mechanism of rationally design and construct advanced systems that can effectively selectively drive NO3RR. There are several natural enzymes incorporate molybdenum (Mo) activate NO3–. Based on this, cadmium (Cd) single-atom anchored Mo2TiC2Tx electrocatalyst (referred CdSA-Mo2TiC2Tx) through NO3RR generate NH3 was designed demonstrated. In an H-type electrolysis cell at current density 42.5 mA cm–2, had Faradaic efficiency >95% impressive yield rate 48.5 mg h–1 cm–2. Moreover, conversion NO3– CdSA-Mo2TiC2Tx surface further revealed by operando attenuated total reflection Fourier-transform infrared spectroscopy electrochemical differential mass spectrometer. significantly outperformed well reported state-of-the-art catalysts. Density functional theory calculations decreased ability d-p orbital hybridize with NH3* intermediates, thereby decreasing activation energy potential-determining step. This work not only highlights application prospects heavy metal catalysts in but also provides examples bio-inspired electrocatalysts synthesis NH3.

Language: Английский

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