Understanding the Dynamic Evolution of Active Sites among Single Atoms, Clusters, and Nanoparticles DOI Open Access

Hongchen Yang,

Pengfei Duan, Zechao Zhuang

et al.

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

Published: Jan. 2, 2025

Abstract Catalysis remains a cornerstone of chemical research, with the active sites catalysts being crucial for their functionality. Identifying sites, particularly during reaction process, is elucidating relationship between catalyst's structure and its catalytic property. However, dynamic evolution within heterogeneous metal presents substantial challenge accurately pinpointing real sites. The advent in situ operando characterization techniques has illuminated path toward understanding changes offering robust scientific evidence to support rational design catalysts. There pressing need comprehensive review that systematically explores among single atoms, clusters, nanoparticles as utilizing techniques. This aims delineate effects various factors on nanoparticles. Moreover, several are elaborated emphases tracking linking them properties. Finally, it discusses challenges future perspectives identifying process advancing

Language: Английский

Tailoring Oxygen Reduction Reaction Kinetics of Fe−N−C Catalyst via Spin Manipulation for Efficient Zinc–Air Batteries DOI
Huiwen Zhang, Hsiao‐Chien Chen,

Solmaz Feizpoor

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(25)

Published: April 9, 2024

The interaction between oxygen species and metal sites of various orbitals exhibits intimate correlation with the reduction reaction (ORR) kinetics. Herein, a new approach for boosting inherent ORR activity atomically dispersed Fe-N-C matrix is represented by implanting Fe atomic clusters nearby. as-prepared catalyst delivers excellent half-wave potentials 0.78 0.90 V in acidic alkaline solutions, respectively. decent can also be validated from high-performance rechargeable Zn-air battery. experiments density functional theory calculations reveal that electron spin-state monodispersed active transferred low spin (LS, t

Language: Английский

Citations

106
Designing 3d Transition Metal Cation-Doped MRuOx As Durable Acidic Oxygen Evolution Electrocatalysts for PEM Water Electrolyzers DOI
Panpan Sun, Zelong Qiao,

Xiaobin Dong

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(22), P. 15515 - 15524

Published: May 24, 2024

The continuous dissolution and oxidation of active sites in Ru-based electrocatalysts have greatly hindered their practical application proton exchange membrane water electrolyzers (PEMWE). In this work, we first used density functional theory (DFT) to calculate the energy Ru 3d transition metal-doped MRuOx (M = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn) evaluate stability for acidic oxygen evolution reaction (OER) screen out ZnRuOx as best candidate. To confirm theoretical predictions, experimentally synthesized these materials found that indeed displays robust OER with a negligible decay η10 after 15 000 CV cycles. Of importance, using anode, PEMWE can run stably 120 h at 200 mA cm–2. We also further uncover mechanism ZnRuOx, i.e., Zn atoms doped outside nanocrystal would form "Zn-rich" shell, which effectively shortened average Ru–O bond lengths strengthen interaction therefore boosted intrinsic OER. short, work not only provides new study paradigm DFT calculations guide experimental synthesis but offers proof-of-concept metal dopants RuO2 stabilizer universal principle develop high-durability catalysts PEMWE.

Language: Английский

Citations

64
Cascade Dual Sites Modulate Local CO Coverage and Hydrogen-Binding Strength to Boost CO2 Electroreduction to Ethylene DOI
Junjun Li, Yu Chen, Bingqing Yao

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(8), P. 5693 - 5701

Published: Feb. 9, 2024

Rationally modulating the binding strength of reaction intermediates on surface sites copper-based catalysts could facilitate C–C coupling to generate multicarbon products in an electrochemical CO2 reduction reaction. Herein, theoretical calculations reveal that cascade Ag–Cu dual synergistically increase local CO coverage and lower kinetic barrier for protonation, leading enhanced asymmetric C2H4. As a proof concept, Cu3N-Ag nanocubes (NCs) with Ag located partial Cu Cu3N unit center are successfully synthesized. The Faraday efficiency current density C2H4 over NCs 7.8 9.0 times those NCs, respectively. In situ spectroscopies combined confirm produce promote *COCHO, significantly enhancing generation Our work provides new insights into catalysis strategy at atomic scale boosting products.

Language: Английский

Citations

60
One-step electrodeposition synthesis of NiFePS on carbon cloth as self-supported electrodes for electrochemical overall water splitting DOI

Yuwei Gui,

Zhetong Liu,

Xiangbo Feng

et al.

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 673, P. 444 - 452

Published: June 12, 2024

Language: Английский

Citations

51
Single‐atom materials: The application in energy conversion DOI Creative Commons
Chenxi Zhu, Jiarui Yang, Jiangwei Zhang

et al.

Interdisciplinary materials, Journal Year: 2024, Volume and Issue: 3(1), P. 74 - 86

Published: Jan. 1, 2024

Abstract Single‐atom materials (SAMs) have become one of the most important power sources to push field energy conversion forward. Among main types energy, including thermal electrical solar and biomass SAMs realized ultra‐high efficiency show an appealing future in practical application. More than high activity, uniform active sites also provide a convincible model for chemists design comprehend mechanism behind phenomenon. Therefore, we presented insightful review application single‐atom material conversion. The challenges (e.g., accurate synthesis application) directions machine learning efficient design) applications are included, aiming guidance research next step.

Language: Английский

Citations

46
Spatial configuration of Fe–Co dual-sites boosting catalytic intermediates coupling toward oxygen evolution reaction DOI Creative Commons

Taiyan Zhang,

Jingjing Jiang, Wenming Sun

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2024, Volume and Issue: 121(6)

Published: Jan. 31, 2024

Oxygen evolution reaction (OER) is the pivotal obstacle of water splitting for hydrogen production. Dual-sites catalysts (DSCs) are considered exceeding single-site due to preternatural synergetic effects two metals in OER. However, appointing specific spatial configuration dual-sites toward more efficient catalysis still remains a challenge. Herein, we constructed configurations Fe-Co dual-sites: stereo sites (stereo-Fe-Co DSC) and planar (planar-Fe-Co DSC). Remarkably, planar-Fe-Co DSC has excellent OER performance superior stereo-Fe-Co DSC. DFT calculations experiments including isotope differential electrochemical mass spectrometry, situ infrared spectroscopy, Raman reveal *O intermediates can be directly coupled form *O-O* rather than *OOH by both DSCs, which could overcome limitation four electron transfer steps Especially, proper distance steric direction benefit cooperation dual dehydrogenate into rate-determining step. This work provides valuable insights support further research development dual-site catalysts.

Language: Английский

Citations

46
Pd–Mn/NC Dual Single-Atomic Sites with Hollow Mesopores for the Highly Efficient Semihydrogenation of Phenylacetylene DOI
Huan Liu, Peng Zhu, Da Yang

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(3), P. 2132 - 2140

Published: Jan. 16, 2024

The direct pyrolysis of metal-zeolite imidazolate frameworks (M-ZIFs) has been widely recognized as the predominant approach for synthesizing atomically dispersed metal–nitrogen-carbon single-atom catalysts (M/NC-SACs), which have exhibited exceptional activity and selectivity in semihydrogenation acetylene. However, due to weak adsorption reactants on single site restricted molecular diffusion, large organic molecules (e.g., phenylacetylene) was greatly limited M/NC-SACs. In this work, a dual catalyst (h–Pd-Mn/NC) with hollow mesopores designed prepared using general host–guest strategy. Taking phenylacetylene an example, ultrahigh selectivity, achieved turnover frequency 218 molC═CmolPd–1 min–1, 16-fold higher than that commercial Lindlar catalyst. maintained high even after 5 cycles usage. superior h–Pd-Mn/NC attributed 4.0 nm mesopore interface catalyst, enhanced diffusion macromolecular products. Particularly, introduction Mn electronegativity could drive electron transfer from adjacent Pd sites regulate electronic structure sites. Meanwhile, strong coupling Pd–Mn pairs d-electron domination near Fermi level promoted H2 active sites, thereby reducing energy barrier phenylacetylene.

Language: Английский

Citations

41
Tuning the Local Environment of Pt Species at CNT@MO2–x (M = Sn and Ce) Heterointerfaces for Boosted Alkaline Hydrogen Evolution DOI
Changan Zhou, Kui Ma, Zechao Zhuang

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(31), P. 21453 - 21465

Published: July 25, 2024

As the most promising hydrogen evolution reaction (HER) electrocatalysts, platinum (Pt)-based catalysts still struggle with sluggish kinetics and expensive costs in alkaline media. Herein, we accelerate by optimizing local environment of Pt species metal oxide heterointerfaces. The well-dispersed PtRu bimetallic clusters adjacent MO2–x (M = Sn Ce) on carbon nanotubes (PtRu/CNT@MO2–x) are demonstrated to be a potential electrocatalyst for HER, exhibiting an overpotential only 75 mV at 100 mA cm–2 1 M KOH. excellent mass activity 12.3 μg–1Pt+Ru specific 32.0 cm–2ECSA 70 56 64 times higher than those commercial Pt/C. Experimental theoretical investigations reveal that heterointerfaces between can simultaneously promote H2O adsorption activation, while modification Ru further optimizes H dissociation energy barriers. Then, matching accelerated elementary steps achieved superb generation This work provides new insight into catalytic design optimize obtaining ideal HER performance.

Language: Английский

Citations

34
Efficient Hydrogen Generation from Ammonia Borane Hydrolysis on a Tandem Ruthenium–Platinum–Titanium Catalyst DOI

Shuyan Guan,

Zhenluo Yuan,

Shiqian Zhao

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(33)

Published: May 28, 2024

Hydrolysis of ammonia borane (NH

Language: Английский

Citations

30
Tandem catalysis in electrocatalytic nitrate reduction: Unlocking efficiency and mechanism DOI Creative Commons
Ziyang Wu, Yanhui Song,

Haocheng Guo

et al.

Interdisciplinary materials, Journal Year: 2024, Volume and Issue: 3(2), P. 245 - 269

Published: Feb. 28, 2024

Abstract The electrochemical nitrate reduction reaction (NO 3 RR) holds promise for ecofriendly removal. However, the challenge of achieving high selectivity and efficiency in electrocatalyst systems still significantly hampers mechanism understanding large‐scale application. Tandem catalysts, comprising multiple catalytic components working synergistically, offer promising potential improving NO RR. This review highlights recent progress designing tandem catalysts RR, including noble metal‐related system, transition metal electrocatalysts, pulsed electrocatalysis strategies. Specifically, optimization active sites, interface engineering, synergistic effects between catalyst components, various situ technologies, theory simulations are discussed detail. Challenges opportunities development scaling up RR further discussed, such as stability, durability, mechanisms. By outlining possible solutions future design, this aims to open avenues efficient comprehensive insights into mechanisms energy sustainability environmental safety.

Language: Английский

Citations

29