Active phase discovery in heterogeneous catalysis via topology-guided sampling and machine learning DOI Creative Commons

Shisheng Zheng,

Ximing Zhang,

Heng-Su Liu

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: March 14, 2025

Understanding active phases across interfaces, interphases, and even within the bulk under varying external conditions environmental species is critical for advancing heterogeneous catalysis. Describing these through computational models faces challenges in generation calculation of a vast array atomic configurations. Here, we present framework automatic efficient exploration phases. This approach utilizes topology-based algorithm leveraging persistent homology to systematically sample configurations diverse coordination environments material morphologies. Simultaneously, machine learning force fields enable rapid computations. We demonstrate effectiveness this two systems: hydrogen absorption Pd, where penetrates subsurface layers bulk, inducing "hex" reconstruction CO2 electroreduction, explored 50,000 sampled configurations; oxidation dynamics Pt clusters, oxygen incorporation renders clusters less during reduction reactions, investigated 100,000 In both cases, predicted their impacts on catalytic mechanisms closely align with previous experimental observations, indicating that proposed strategy can model complex systems discovery specific conditions. Discovering heterocatalysis entails configuration sampling optimization. authors developed based topology effectively explore structures, applied electroreduction Oxygen Reduction Reaction

Language: Английский

Bridging the complexity gap in computational heterogeneous catalysis with machine learning DOI
Tianyou Mou, Hemanth Somarajan Pillai, Siwen Wang

et al.

Nature Catalysis, Journal Year: 2023, Volume and Issue: 6(2), P. 122 - 136

Published: Feb. 23, 2023

Language: Английский

Citations

135
Tailoring acidic microenvironments for carbon-efficient CO2electrolysis over a Ni–N–C catalyst in a membrane electrode assembly electrolyzer DOI
Hefei Li, Haobo Li, Pengfei Wei

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(4), P. 1502 - 1510

Published: Jan. 1, 2023

By tailoring the microenvironments of a Ni–N–C catalyst in an acidic MEA electrolyzer, we achieve CO faradaic efficiency 95% at 500 mA cm −2 , and 2 loss is reduced by 86% 300 pH 0.5, compared to alkaline electrolysis.

Language: Английский

Citations

109
C2+ Selectivity for CO2 Electroreduction on Oxidized Cu-Based Catalysts DOI
Haobo Li,

Yunling Jiang,

Xinyu Li

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(26), P. 14335 - 14344

Published: June 21, 2023

Design for highly selective catalysts CO2 electroreduction to multicarbon (C2+) fuels is pressing and important. There is, however, presently a poor understanding of selectivity toward C2+ species. Here we report the first time method judiciously combined quantum chemical computations, artificial-intelligence (AI) clustering, experiment development model relationship between product composition oxidized Cu-based catalysts. We 1) evidence that Cu surface more significantly facilitates C-C coupling, 2) confirm critical potential condition(s) this oxidation state under different metal doping components viaab initio thermodynamics computation, 3) establish an inverted-volcano experimental Faradaic efficiency using multidimensional scaling (MDS) results based on physical properties dopant elements, 4) demonstrate design electrocatalysts selectively generate product(s) through co-doping strategy early late transition metals. conclude combination theoretical AI can be used practically relationships descriptors complex reactions. Findings will benefit researchers in designing conversions products.

Language: Английский

Citations

93
Covalent triazine frameworks for advanced energy storage: challenges and new opportunities DOI
Peng Xiong, Shilin Zhang, Rui Wang

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(8), P. 3181 - 3213

Published: Jan. 1, 2023

This Review provides a comprehensive overview of recent advancements in CTF materials and CTF-based batteries. The aims to make batteries viable for next-generation high-energy battery systems.

Language: Английский

Citations

83
Activity and Selectivity Roadmap for C–N Electro-Coupling on MXenes DOI
Yiran Jiao, Haobo Li, Yan Jiao

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(28), P. 15572 - 15580

Published: July 6, 2023

Electrochemical coupling between carbon and nitrogen species to generate high-value C-N products, including urea, presents significant economic environmental potentials for addressing the energy crisis. However, this electrocatalysis process still suffers from limited mechanism understanding due complex reaction networks, which restricts development of electrocatalysts beyond trial-and-error practices. In work, we aim improve mechanism. This goal was achieved by constructing activity selectivity landscape on 54 MXene surfaces density functional theory (DFT) calculations. Our results show that step is largely determined *CO adsorption strength (Ead-CO), while relies more co-adsorption *N (Ead-CO Ead-N). Based these findings, propose an ideal catalyst should satisfy moderate stable adsorption. Through machine learning-based approach, data-driven formulas describing relationship Ead-CO Ead-N with atomic physical chemistry features were further identified. identified formula, 162 materials screened without time-consuming DFT Several potential catalysts predicted good performance, such as Ta2W2C3. The candidate then verified study has incorporated learning methods first time provide efficient high-throughput screening method selective electrocatalysts, could be extended a wider range electrocatalytic reactions facilitate green chemical production.

Language: Английский

Citations

57
Recent advancements on designing transition metal-based carbon-supported single atom catalysts for oxygen electrocatalysis: Miles to go for sustainable Zn-air batteries DOI
Srijib Das, Aniruddha Kundu, Tapas Kuila

et al.

Energy storage materials, Journal Year: 2023, Volume and Issue: 61, P. 102890 - 102890

Published: July 18, 2023

Language: Английский

Citations

45
Role of H2O in Catalytic Conversion of C1 Molecules DOI
Lei Jiang, Kongzhai Li, William N. Porter

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(5), P. 2857 - 2875

Published: Jan. 24, 2024

Due to their role in controlling global climate change, the selective conversion of C

Language: Английский

Citations

26
Dynamic Cu0/Cu+ Interface Promotes Acidic CO2 Electroreduction DOI

Yunling Jiang,

Haobo Li, Chaojie Chen

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(11), P. 8310 - 8316

Published: May 13, 2024

Acidic CO2 electroreduction reaction (CO2RR) shows advantages in high carbon utilization efficiency yet encounters great challenges suppressing undesired hydrogen evolution competition and increasing C2+ product selectivity. Although it is known that Cu0/Cu+ interfaces are conducive to C–C coupling processes, the oxidation state of copper cannot be well maintained under strong reductive condition large current electrolysis operation. Herein, we propose an I2 addition involved strategy protect Cu promote dynamic during acidic CO2RR. With electrolyte, a Faraday above 70% can achieved at 0.4–0.6 A cm–2 even low K+ concentration 0.3 M, which comparable those reported performances with almost ten times higher concentrations (2–3 M). This electrolytes significantly avoids salt crystallization transport channel enhance electrolyzer's stability. As proved by surface Pourbaix diagram experimental results, adding excessive into electrolyte boosts generation CuI; also, CuI metallic coexist electrochemical reduction conditions, demonstrating redox loop → exists. The holds key constructing interface, tightly bound adsorption *CO intermediate further promotes process.

Language: Английский

Citations

24
From Characterization to Discovery: Artificial Intelligence, Machine Learning and High-Throughput Experiments for Heterogeneous Catalyst Design DOI
Jorge Benavides-Hernández, Franck Dumeignil

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(15), P. 11749 - 11779

Published: July 24, 2024

This review paper delves into synergistic integration of artificial intelligence (AI) and machine learning (ML) with high-throughput experimentation (HTE) in the field heterogeneous catalysis, presenting a broad spectrum contemporary methodologies innovations. We methodically segmented text three core areas: catalyst characterization, data-driven exploitation, discovery. In characterization part, we outline current prospective techniques used for HTE how AI-driven strategies can streamline or automate their analysis. The exploitation part is divided themes, strategies, that offer flexibility either modular application creation customized solutions. exploration present applications enable areas outside experimentally tested chemical space, incorporating section on computational methods identifying new prospects. concludes by addressing limitations within suggesting possible avenues future research.

Language: Английский

Citations

24
Carbon Support Enhanced Mass Transfer and Metal–Support Interaction Promoted Activation for Low-Concentrated Nitric Oxide Electroreduction to Ammonia DOI

Jinying Meng,

Chuanqi Cheng, Yuting Wang

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(14), P. 10044 - 10051

Published: April 1, 2024

The electrochemical NO reduction reaction (NORR) is a promising approach for both nitrogen cycle regulation and ammonia synthesis. Due to the relatively low concentration of source poor solubility in solution, mass transfer limitation serious but easily overlooked issue. In this work, porous carbon-supported ultrafine Cu clusters grown on nanowire arrays (defined as Cu@Cu/C NWAs) are prepared low-concentration NORR. A high Faradaic efficiency (93.0%) yield rate (1180.5 μg h–1 cm–2) realized NWAs at −0.1 V vs reversible hydrogen electrode (RHE), which far superior those other reported performances under similar conditions. construction carbon support can effectively decrease diffusion kinetics promote coverage subsequent highly effective conversion. Moreover, favorable metal–support interaction between enhances adsorption decreases barrier *HNO formation comparison with that pure NWAs. Overall, whole NORR be fully strengthened concentrations.

Language: Английский

Citations

23