Machine Learning-Enhanced Screening of Single-Atom Alloy Clusters for Nitrogen Reduction Reaction DOI
Arunendu Das, Diptendu Roy, A. Das

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(43), P. 58648 - 58656

Published: Oct. 16, 2024

The electrochemical nitrogen reduction reaction (eNRR) under ambient conditions is a promising method to generate ammonia (NH3), crucial precursor for fertilizers and chemicals, without carbon emissions. Single-atom alloy catalysts (SAACs) have reinvigorated catalytic processes due their high activity, selectivity, efficient use of active atoms. Here, we employed density functional theory (DFT) calculations integrated with machine learning (ML) investigate dodecahedral nanocluster-based SAACs analyzing structure–activity relationships in eNRR. Over 300 were screened all the transition metals as dopants develop an ML model predicting stability performance. Facet sites identified optimal doping positions, particularly late group showing superior activity. Utilizing DFT+ML, 8 highly suitable Interestingly, number valence d-electrons proved screening eNRR These exhibited low activity hydrogen evolution reaction, further enhancing suitability This successful ML-driven approach accelerates catalyst design discovery, holding significant practical implications.

Language: Английский

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
Mapping the Binary Covalent Alloy Space to Pursue Superior Nitrogen Reduction Reaction Catalysts DOI

Cooper Tezak,

Sophie Gerits,

Benjamin Rich

et al.

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

Published: May 5, 2024

Abstract The electrochemical nitrogen reduction reaction (NRR) has the potential to decarbonize industrial ammonia production. However, NRR poor activity and selectivity versus competing hydrogen evolution for catalysts that adhere scaling relations. Overcoming limitations imposed by relations requires more complex catalyst materials, however, evaluating materials beyond simple metal systems is a large combinatorial problem an improved understanding of electrocatalyst surface rationally guide discovery superior catalysts. study uses grand canonical density functional theory uncover trends on disparate set binary covalent alloys (BCA) with variable compositions active‐site geometries. studied BCAs generally follow relations, albeit larger variance several significantly break scaling. early‐ mid‐transition metals tend lie near volcano peak activate N 2 triple bond via side‐on binding configuration. Trends in BCA space cannot be readily predicted using electronic descriptors, which ascribed geometric variability surfaces. It anticipated these findings will provide foundation rational design electrocatalysts increasing material complexity.

Language: Английский

Citations

12
Electronic structure modulation of high entropy materials for advanced electrocatalysis DOI Creative Commons
Luoluo Qi, Jingqi Guan

Green Energy & Environment, Journal Year: 2024, Volume and Issue: unknown

Published: July 1, 2024

High-entropy materials (HEMs) have managed to make their mark in the field of electrocatalysis. The flexibly adjustable component, unique configuration and proprietary core effect endow HEMs with excellent functional feature, superior stability fast reaction kinetics. Recently, relationship between compositions structures high-entropy catalysts electrocatalytic performances has been extensively investigated. Based on this motivation, we comprehensively systematically summarize HEMs, outline intrinsic properties electrochemical advantages, generalize current state-of-the-art synthetic methods, analyze active centers conjunction characterization techniques, utilize theoretical research conduct a high-throughput screening targeted catalyst exploration mechanisms, importantly, focus specially applications propose strategies for regulating electronic structure accelerate kinetics, including morphological control, defect engineering, element regulation, strain engineering so forth. Finally, provide our personal views challenges further technical improvements catalysts. This work can valuable guidance future electrocatalysts.

Language: Английский

Citations

8
Insights into Electrochemical CO2 Reduction on Metallic and Oxidized Tin Using Grand-Canonical DFT and In Situ ATR-SEIRA Spectroscopy DOI Creative Commons
Todd N. Whittaker, Yuval Fishler, Jacob M. Clary

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(11), P. 8353 - 8365

Published: May 14, 2024

Electrochemical CO2 reduction (CO2R) to formate is an attractive carbon emissions mitigation strategy due the existing market and price for formic acid. Tin effective electrocatalyst CO2R formate, but underlying reaction mechanism whether active phase of tin metallic or oxidized during openly debated. In this report, we used grand-canonical density functional theory attenuated total reflection surface-enhanced infrared absorption spectroscopy identify differences in vibrational signatures surface species on fully surfaces. Our results show that feasible both tin. We propose key difference between each termination catalyzed by surfaces limited electrochemical activation CO2, whereas slow reductive desorption formate. While exact degree oxidation unlikely be either oxidized, study highlights limiting behavior these two lays out features our predict will promote rapid catalysis. Additionally, highlight power integrating high-fidelity quantum mechanical modeling spectroscopic measurements elucidate intricate electrocatalytic pathways.

Language: Английский

Citations

7
Selective Nitrogen Reduction Reaction on Single-Atom Centers of Molybdenum-Based MXenes by Pulsing the Electrochemical Potential DOI
Divya Singh, Samad Razzaq,

Shohreh Faridi

et al.

Published: Jan. 1, 2025

Electrocatalytic reduction of dinitrogen is a promising route for sustainable production ammonia, although the selectivity challenge competing nitrogen (NRR) and hydrogen evolution reactions in aqueous electrolytes has not yet been solved. Single-atom catalysts (SACs) offer hope bridging this gap because they exhibit unique electronic structure reactivity catalytic transformations compared to conventional bulk materials. In addition, potential pulse experiments have shown that promote formation kinetically unfavorable products by efficiently modulating electrolyte at solid-liquid interface. So far, combination SACs NRR mutually exclusive, since are likely be degraded during anodic due metal dissolution. Using density functional theory calculations grand canonical framework, we demonstrate present communication molybdenum-based MXenes able overcome limitation: traditional SACs, form single-atom centers pulse, their SAC-like allows directed ammonia instead gaseous cathodic pulse. Our study paves way development high-performance materials with in-situ formed sites enable advances selective under applied bias.

Language: Английский

Citations

0
Advances in CO2 Reduction on Bulk and Two-Dimensional Electrocatalysts: From First Principles to Experimental Outcomes DOI
Raghavan Rajagopalan, Shivam Chaturvedi, Neeru Chaudhary

et al.

Current Opinion in Electrochemistry, Journal Year: 2025, Volume and Issue: unknown, P. 101668 - 101668

Published: Feb. 1, 2025

Language: Английский

Citations

0
Tunable N2 Fixation Enabled by Ferroelectric Switching in Doped Graphene/In2Se3 Dual-Atom Catalysts DOI Creative Commons

Mohammad Amin Akhound,

Maryam Soleimani, Mahdi Pourfath

et al.

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 27, 2025

The electrochemical nitrogen reduction reaction (NRR) provides a sustainable alternative to ammonia synthesis. However, the development of catalysts with high activity and selectivity under ambient conditions remains significant challenge. In this work, we propose class dual-atom (DACs), consisting two metal atoms embedded in nitrogen-doped porous graphene (M2NPG) supported on ferroelectric α-In2Se3 monolayer. Using density functional theory (DFT) calculations, explore effect polarization switching structural stability, catalytic performance, mechanisms these DACs. By computationally screening 27 as active sites, identify four promising candidates (V, Co, Ru, Ta) V2NPG@In2Se3 standing out due its exceptional properties. precise control NRR pathways, along tunable limiting potentials selective product formation, can be achieved through combination low potential, abundant behavior, against hydrogen evolution (HER) highlights potential traditional single-atom catalysts. This work demonstrates versatile strategy for integrating DACs materials, offering valuable insights into designing next-generation beyond.

Language: Английский

Citations

0
Selective nitrogen reduction reaction on single-atom centers of molybdenum-based MXenes by pulsing the electrochemical potential DOI Creative Commons
Divya Singh, Samad Razzaq,

Shohreh Faridi

et al.

Materials Today, Journal Year: 2025, Volume and Issue: unknown

Published: April 1, 2025

Language: Английский

Citations

0
Electrochemical nitrogen reduction reaction on anchored SnS2 nanosheets with TM2 dimers DOI

Ruixin Xu,

Shiqian Cao,

Tingting Bo

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 660, P. 290 - 301

Published: Jan. 19, 2024

Language: Английский

Citations

2
Impact of Vacancy Defects on Electrochemical Nitrogen Reduction Reaction Performance of MXenes DOI
Hardik L. Kagdada, Ankit Jain

ChemPhysChem, Journal Year: 2024, Volume and Issue: 25(10)

Published: Feb. 19, 2024

Abstract We investigated electrochemical nitrogen reduction reaction (eNRR) on MXenes consisting of the vacancy defects in functional layer using density theory calculations. considered Mo 2 C, W N, and N with F, O functionalization distal alternative associative pathways. analyzed these for eNRR based adsorption energy, NH 3 desorption NRR selectivity, limiting potential. While we find that most surfaces are more favorable compared to hydrogen evolution, also have strong binding (>−1.0 eV) thus will be covered during operating conditions. Amongst all MXenes, only NF is found a low energy along overpotential selectivity towards eNRR. The obtained superior those reported pristine as well functionalized MXenes.

Language: Английский

Citations

2