Density Functional Theory Investigation on the Nitrogen Reduction Mechanism in Two-Dimensional Transition-Metal Boride with Ordered Metal Vacancies DOI
Linghuan Ma, Xianfei Chen,

Yi Huang

et al.

Langmuir, Journal Year: 2024, Volume and Issue: 40(28), P. 14355 - 14367

Published: July 4, 2024

The creation of ordered collective vacancies in experiment proves challenging within a two-dimensional lattice, resulting limited understanding their impact on catalyst performance. Motivated by the successful experimental synthesis monolayer molybdenum borides with precisely metal [Zhou et al.

Language: Английский

High‐Throughput Screening of Electrocatalysts for Nitrogen Reduction Reactions Accelerated by Interpretable Intrinsic Descriptor DOI
Xiaoyun Lin, Yongtao Wang, Xin Chang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(19)

Published: March 9, 2023

Developing easily accessible descriptors is crucial but challenging to rationally design single-atom catalysts (SACs). This paper describes a simple and interpretable activity descriptor, which obtained from the atomic databases. The defined descriptor proves accelerate high-throughput screening of more than 700 graphene-based SACs without computations, universal for 3-5d transition metals C/N/P/B/O-based coordination environments. Meanwhile, analytical formula this reveals structure-activity relationship at molecular orbital level. Using electrochemical nitrogen reduction as an example, descriptor's guidance role has been experimentally validated by 13 previous reports well our synthesized 4 SACs. Orderly combining machine learning with physical insights, work provides new generalized strategy low-cost while comprehensive understanding structure-mechanism-activity relationship.

Language: Английский

Citations

52
Progress in Single/Multi Atoms and 2D‐Nanomaterials for Electro/Photocatalytic Nitrogen Reduction: Experimental, Computational and Machine Leaning Developments DOI
Aditya Narayan Singh, Rohit Anand, Mohammad Zafari

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(28)

Published: Feb. 11, 2024

Abstract The conversion of atmospheric nitrogen (N 2 ) into ammonia (NH 3 ), known as fixation, plays a crucial role in sustaining life on Earth, facing innovation with electrocatalytic and photocatalytic methods. These approaches promise gentler conversions from to ammonia, diverging the energy‐intensive Haber‐Bosch process, which requires complex plant infrastructure. Vitality lies eco‐friendly, cost‐effective, energy‐efficient pathways. challenge is that electrocatalysts photocatalysts for reduction have shown low Faraday efficiency, hampered by hydrogen evolution. This work delves recent strides electro/photo‐catalytic fixation/reduction, deciphering mechanisms, catalysts, prospects. By unveiling core principles steering these processes, it dissects efficiency drivers. Experimental theoretical studies, ranging density functional calculations/simulations machine learning‐based catalyst screening, mark path toward highly efficient including single/multi‐atom catalysts embedded 2D materials. journey explores diverse assessing their performance, spotlighting emerging nanomaterials, heterostructures, co‐catalyst techniques. Perspectives future directions potential applications fixation/reduction are offered, emphasizing sustainable management implications global agriculture environmental sustainability.

Language: Английский

Citations

31
Theoretical design toward highly efficient single-atom catalysts for nitrogen reduction by regulating the “acceptance-donation” mechanism DOI Open Access
Yaqin Zhang, Ninggui Ma, Yuhang Wang

et al.

Applied Surface Science, Journal Year: 2023, Volume and Issue: 623, P. 156827 - 156827

Published: Feb. 23, 2023

Language: Английский

Citations

26
The Electron‐Rich Interface Regulated MBene by S‐Bridge Guided to Enhance Nitrogen Fixation under Environmental Conditions DOI Open Access

Kun Cheng,

Shaobin Li,

Qingyu Cheng

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 15, 2024

Abstract The underutilization of active sites limits the performance enhancement 2D transition metal boride (MBene) in electrocatalytic nitrogen reduction reaction (NRR). Herein, a highly efficient NRR electrocatalyst with S atoms bridging Fe and Mo on surface MBene is successfully constructed by using an site electron optimization strategy, which increases charge density around enhances activation ability catalyst to N 2 molecules. It noteworthy that FeS ‐MBene demonstrates low intrinsic potential for (−0.2 V vs RHE). more favorable adsorption comparison hydrogen atoms, thereby it can effectively inhibit evolution (HER). Under −0.2 versus RHE, ammonia yield rate 37.13 ± 1.31 µg h −1 mg , FE 55.97 2.63%. Density functional theory (DFT) calculations demonstrate serves as . formation heterostructure transfer, resulting becoming electron‐rich state favor subsequent hydrogenation steps. This work offers significant insights into design utilization MBene‐based catalysts NRR.

Language: Английский

Citations

15
The rational co-doping strategy of transition metal and non-metal atoms on g-CN for highly efficient hydrogen evolution by DFT and machine learning DOI
Yang Yu, Xin Zhao, Tianyun Liu

et al.

International Journal of Hydrogen Energy, Journal Year: 2024, Volume and Issue: 56, P. 949 - 958

Published: Jan. 1, 2024

Language: Английский

Citations

14
2D, Metal‐Free Electrocatalysts for the Nitrogen Reduction Reaction DOI Creative Commons
Chuangwei Liu,

Ang Tian,

Qinye Li

et al.

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 33(9)

Published: Dec. 16, 2022

Abstract Environmentally friendly ammonia production is important for addressing the carbon emissions and substantial energy consumption that are currently associated with chemical industry. In recent decades, many achievements made in this area; however, low yield, poor selectivity, unsatisfactory Faradaic efficiency hinder large‐scale applications. 2D, metal‐free electrocatalysts stand out from other candidates because of their physical, electronic, properties. study, developments 2D‐based electrochemical materials converting dinitrogen into ambient conditions systematically reviewed. First, unique progress challenges on novel 2D nitrogen reduction reaction summarized. Then, various synthetic strategies influence these methods have intrinsic material performance highlighted. Last, by comparing current engineering strategies, tests, computational calculations, opportunities, critical issues, scientific nanomaterials as stable, efficient catalysts, analyzed. On basis comparison, technology solutions provided rational principles future studies proposed.

Language: Английский

Citations

36
Single-atom catalytic N2 fixation with integrated descriptors on a novel π-π conjugated graphitic carbon nitride (g-C13N15) platform obtained by self-doping design: Prediction of ultrahigh activity and desirable selectivity DOI
Yali Lu, Chunyao Fang, Qiang Zhang

et al.

Journal of Power Sources, Journal Year: 2024, Volume and Issue: 595, P. 234030 - 234030

Published: Jan. 11, 2024

Language: Английский

Citations

7
2D conductive metal–organic frameworks for NO electrochemical reduction: a first-principles study DOI
Xing Chen, Xiangyu Zhu, Zhiyuan Xia

et al.

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(35), P. 23612 - 23621

Published: Jan. 1, 2024

Designing flexible single-atom catalysts with tunable centers and coordination environments is crucial for highly active selective electrochemical catalysis.

Language: Английский

Citations

7
The role of central heteroatom in electrochemical nitrogen reduction catalyzed by polyoxometalate-supported single-atom catalyst DOI

Linghui Lin,

Fenfei Wei, Rong Jiang

et al.

Nano Research, Journal Year: 2022, Volume and Issue: 16(1), P. 309 - 317

Published: Aug. 17, 2022

Language: Английский

Citations

28
High-Throughput Screening of Transition-Metal-Atom-Embedded Parallel Tetracyanoethylene 2D Networks as Single-Atom Electrocatalysts for Ammonia Synthesis and Its Underlying Microscopic Mechanisms DOI
Dan Deng, Bingyi Song, Cong Li

et al.

The Journal of Physical Chemistry C, Journal Year: 2022, Volume and Issue: 126(49), P. 20816 - 20830

Published: Dec. 2, 2022

Electrosynthesis of ammonia under mild conditions has been impeded by the lack high-performance electrocatalysts. Inspired high activity and selectivity single-atom catalysts (SACs) with maximum atom utilization, we systematically explored a new class two-dimensional SACs formed embedding 30 types transition metals (TMs) in (2D) parallel patterning tetracyanoethylene (TCNE) networks (labeled as p-TM[TCNE], p means parallel) for nitrogen reduction reaction (NRR) through combination high-throughput screening density functional theory calculations. Three p-TM[TCNE] (TM = Mo, Nb, Ti) stand out catalytic selectivity. The full path search demonstrates that these three prefer distal mechanism, among which p-Mo[TCNE] lowest limiting potential −0.36 V. origin might be ascribed to joint effects from exposed active sites 2D planar structures, stability metallic properties catalysts, efficient charge transfer between adsorbed N2 sites. Interestingly, performance can correlated well magnetic moment metal, indicates could used an descriptor NRR. This work will shed some light on rational design NRR stimulate further efforts both experiment this field.

Language: Английский

Citations

28