High-Throughput Screening of Synergistic Transition Metal Dual-Atom Catalysts for Efficient Nitrogen Fixation

Nano Letters, Journal Year: 2021, Volume and Issue: 21(4), P. 1871 - 1878

Published: Feb. 15, 2021

Great enthusiasm in single-atom catalysts (SACs) for the nitrogen reduction reaction (NRR) has been aroused by discovery of metal–Nx as a promising catalytic center. However, poor activity and low selectivity available SACs are far away from industrial requirement. Through first-principles high-throughput screening, we find that Fe–Fe distributed on graphite carbon nitride (Fe2/g-CN) can manipulate binding strength target species (compromises ability to adsorb N2H NH2), therefore achieving best NRR performance among 23 transition metal (TM) centers. Our results show Fe2/g-CN achieves high theoretical Faradaic efficiency 100% and, impressively, lowest limiting potential −0.13 V. Particularly, multiple-level descriptors shed light origin activity, fast prescreening various candidates. predictions not only accelerate ammonia synthesis but also contribute further elucidate structure–performance correlations.

Language: Английский

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Electronic Modulation of Non‐van der Waals 2D Electrocatalysts for Efficient Energy Conversion

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(26)

Published: May 25, 2021

Abstract The exploration of efficient electrocatalysts for energy conversion is important green development. Owing to their high surface areas and unusual electronic structure, 2D have attracted increasing interest. Among them, non‐van der Waals (non‐vdW) materials with numerous chemical bonds in all three dimensions novel properties beyond those vdW been studied increasingly over the past decades. Herein, progress non‐vdW critically reviewed, a special emphasis on structure modulation. Strategies heteroatom doping, vacancy engineering, pore creation, alloying, heterostructure engineering are analyzed tuning structures achieving intrinsically enhanced electrocatalytic performances. Lastly, roadmap future development provided from material, mechanism, performance viewpoints.

Language: Английский

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“More is Different:” Synergistic Effect and Structural Engineering in Double‐Atom Catalysts

Advanced Functional Materials, Journal Year: 2020, Volume and Issue: 31(3)

Published: Nov. 16, 2020

Abstract Double‐atom catalysts (DACs) have emerged as a novel frontier in heterogeneous catalysis because the synergistic effect between adjacent active sites can promote their catalytic activity while maintaining high atomic utilization efficiency, good selectivity, and stability originating from atomically dispersed nature. In this review, recent progress both experimental theoretical research on DACs for various reactions is focused. Specifically, central tasks design of DACs—manipulating engineering electronic structures catalysts—are systematically reviewed, along with prevailing experimental, characterization, computational modeling approaches. Furthermore, practical applications water splitting, oxygen reduction reaction, nitrogen carbon dioxide reaction are addressed. Finally, future challenges summarized an outlook further investigations toward high‐performance energy environmental provided.

Language: Английский

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Rational Design of Single‐Atom Site Electrocatalysts: From Theoretical Understandings to Practical Applications

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(34)

Published: July 8, 2021

Atomically dispersed metal-based electrocatalysts have attracted increasing attention due to their nearly 100% atomic utilization and excellent catalytic performance. However, current fundamental comprehension summaries reveal the underlying relationship between single-atom site (SACs) corresponding application are rarely reported. Herein, understandings intrinsic mechanisms SACs electrocatalytic applications systemically summarized. Different preparation strategies presented synthetic with engineering well-defined on basis of theoretical principle (size effect, metal-support interactions, electronic structure coordination environment effect). Then, an overview is presented, including oxygen reduction reaction, hydrogen evolution oxidation small organic molecules, carbon dioxide nitrogen reaction. The structure-performance reactions also discussed in depth expound enhancement mechanisms. Finally, a summary provided perspective supplied demonstrate challenges opportunities for rational designing, synthesizing, modulating advanced toward reactions.

Language: Английский

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Gradient Hydrogen Migration Modulated with Self-Adapting S Vacancy in Copper-Doped ZnIn₂S₄ Nanosheet for Photocatalytic Hydrogen Evolution

ACS Nano, Journal Year: 2021, Volume and Issue: 15(9), P. 15238 - 15248

Published: Aug. 19, 2021

It is a challenge to regulate charge flow synergistically at the atomic level modulate gradient hydrogen migration (H migration) for boosting photocatalytic evolution. Herein, self-adapting S vacancy (Vs) induced with Cu introduction into ZnIn2S4 nanosheets was fabricated elaborately, which can tune separation and construct channel H migration. Detailed experimental results theoretical simulations uncover behavior mechanism of Vs generation after substituting Zn atom tendentiously. Cu–S bond shrinkage Zn–S distortion are presented around areas. Besides, by lowers internal electric field restrain electron transmission between layers, enriched on area because lower surface electrostatic potential. Atomic show synergistic effect regulating regional due dopant being hole trap an trap. The channels ΔGH0 constructed different sites, modulated Vs. Gradient driven photothermal occurs identical without striding across heterogeneous interface, valid pathway resistance H2 release. Ultimately, 5 mol % confined in achieves optimum evolution activity 9.8647 mmol g–1 h–1, 14.8 times higher than 0.6640 h–1 ZnIn2S4, apparent quantum efficiency reaches 37.11% 420 nm. This work demonstrates substitution provides cognition deeply.

Language: Английский

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