Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application

Advanced Materials, Год журнала: 2023, Номер 35(31)

Опубликована: Фев. 23, 2023

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric electronic uncovering structure-property relationships of single/dual-metal confront with grand challenges. Herein, this review summarizes latest progress in microenvironment engineering single/dual-atom sites via a comprehensive comparison single-atom catalyst (SACs) dual-atom catalysts (DACs) term design principles, modulation strategy, theoretical understanding structure-performance correlations. Subsequently, recent advances several typical electrocatalysis process are discussed to get general reaction mechanisms finely-tuned SACs DACs. Finally, full-scaled summaries challenges prospects given for This will provide new inspiration development atomically dispersed electrocatalytic application.

Язык: Английский

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Engineering Heterogeneous Catalysis with Strong Metal–Support Interactions: Characterization, Theory and Manipulation

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(4)

Опубликована: Окт. 26, 2022

Strong metal-support interactions (SMSI) represent a classic yet fast-growing area in catalysis research. The SMSI phenomenon results the encapsulation and stabilization of metal nanoparticles (NPs) with support material that significantly impacts catalytic performance through regulation interfacial interactions. Engineering provides promising approach to steer various chemical processes, which serves as an effective tool tackle energy environmental challenges. Our Minireview covers characterization, theory, activity, dependence on structure inducing environment phenomena. By providing overview outlook cutting-edge techniques this multidisciplinary research field, we not only want provide insights into further exploitation catalysis, but also hope inspire rational designs characterization broad field science physical chemistry.

Язык: Английский

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Review of Carbon Support Coordination Environments for Single Metal Atom Electrocatalysts (SACS)

Advanced Materials, Год журнала: 2023, Номер 36(1)

Опубликована: Апрель 20, 2023

This topical review focuses on the distinct role of carbon support coordination environment single-atom catalysts (SACs) for electrocatalysis. The article begins with an overview atomic configurations in SACs, including a discussion advanced characterization techniques and simulation used understanding active sites. A summary key electrocatalysis applications is then provided. These processes are oxygen reduction reaction (ORR), evolution (OER), hydrogen (HER), nitrogen (NRR), dioxide (CO

Язык: Английский

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Synthesis and modification strategies of g-C3N4 nanosheets for photocatalytic applications

Advanced Powder Materials, Год журнала: 2023, Номер 3(1), С. 100150 - 100150

Опубликована: Июль 5, 2023

Graphitic carbon nitride nanosheets (CNNs) become the most promising member in family benefitted from their two-dimensional structural features. Recently, great endeavors have been made synthesis and modification of CNNs to improve photocatalytic properties, many exciting progresses gained. In order elucidate fundamentals based catalysts provide insights into rational design photocatalysis system, we describe recent progress preparation strategies applications this review. Firstly, physicochemical properties are briefly introduced. Secondly, approaches reviewed, including top-down stripping (thermal, gas, liquid, composite stripping) bottom-up precursor molecules (solvothermal, template, supramolecular self-assembly method). Subsequently, on years discussed, crystal structure design, doping, surface functionalization, constructing 2D heterojunction, anchoring single-atom. Then multifunctional g-C3N4 nanosheet materials H2 evolution, O2 overall water splitting, H2O2 production, CO2 reduction, N2 fixation, pollutant removal, organic synthesis, sensing highlighted. Finally, opportunities challenges for development high-performance systems also promising.

Язык: Английский

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Synergies of Adjacent Sites in Atomically Dispersed Ruthenium toward Achieving Stable Hydrogen Evolution

Inorganic Chemistry, Год журнала: 2022, Номер 61(34), С. 13453 - 13461

Опубликована: Авг. 15, 2022

It is a challenge to fabricate atomically dispersed metal clusters in polymeric carbon nitride (PCN) for durable photocatalytic reactions owing the thermodynamic stability limitation. Herein, Ru are implanted into PCN skeleton matrix based on an ionic diffusion and coordination (IDC) strategy, of which improved robust Ru-N bonds formed RuN4 RuN3 configurations. Additionally, as charge transport bridges between two adjacent melon strands efficaciously conquer hydrogen bond restriction facilitate in-plane mobility separation carriers. Moreover, synergistic effect atoms triggered assembled RuN3-RuN4 RuN3-RuN3 significantly decrease adsorption energy. As result, optimal PCN-Ru photocatalyst achieves nearly 6 times higher than evolution (PHE) rate Pt/PCN benchmark maintains long-term stable running 104 h 26 cycles; its overall PHE performance far superior most single supported g-C3N4 photocatalysts reported. The findings here gain new insight preparation structure configuration, reaction mechanism PCN, further stimulates intensive investigations toward developing more efficient PCN-like materials.

Язык: Английский

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Recent Progress of Diatomic Catalysts: General Design Fundamentals and Diversified Catalytic Applications

Small, Год журнала: 2022, Номер 18(46)

Опубликована: Сен. 23, 2022

Abstract In recent years, some experiments and theoretical work have pointed out that diatomic catalysts not only retain the advantages of monoatomic catalysts, but also introduce a variety interactions, which exceed limit catalytic performance can be applied to many fields. Here, interaction between adjacent metal atoms in is elaborated: synergistic effect, spacing enhancement effect (geometric effect), electronic effect. With regard classification characterization various new are classified into four categories: heteronuclear/homonuclear, with/without carbon carriers, their measures introduced explained detail. aspect preparation widely used atomic layer deposition method, metal–organic framework derivative simple ball milling method introduced, with emphasis on formation mechanism catalysts. Finally, effective control strategies key applications electrocatalysis, photocatalysis, thermal catalysis, other fields given.

Язык: Английский

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Single Atom Catalysts for Selective Methane Oxidation to Oxygenates

ACS Nano, Год журнала: 2022, Номер 16(6), С. 8557 - 8618

Опубликована: Май 31, 2022

Direct conversion of methane (CH4) to C1–2 liquid oxygenates is a captivating approach lock carbons in transportable value-added chemicals, while reducing global warming. Existing approaches utilizing the transformation CH4 fuel via tandemized steam reforming and Fischer–Tropsch synthesis are energy capital intensive. Chemocatalytic partial oxidation remains challenging due negligible electron affinity, poor C–H bond polarizability, high activation barrier. Transition-metal stoichiometric catalysts harsh oxidants reaction conditions perform poorly with randomized product distribution. Paradoxically, which active enough break also promote overoxidation, resulting CO2 generation reduced carbon balance. Developing can bonds selectively make useful chemicals at mild vital commercialization. Single atom (SACs) specifically coordinated metal centers on support have displayed intrigued reactivity selectivity for oxidation. SACs significantly reduce induced electrostatic polarization facilitate accelerated rate low temperature. The distinct metal–support interaction stabilize intermediate prevent overoxidation products. present review accounts recent progress field selective oxygenates. chemical nature catalytic sites, effects interaction, stabilization species minimize thoroughly discussed forward-looking perspective improve performance.

Язык: Английский

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Directional Charge Transfer Channels in a Monolithically Integrated Electrode for Photoassisted Overall Water Splitting

ACS Nano, Год журнала: 2023, Номер 17(4), С. 3465 - 3482

Опубликована: Фев. 10, 2023

Photoelectrocatalytic performance of a system is fundamentally determined by the full absorption sunlight and high utilization photoexcited carriers, but efficiency latter largely limited inefficient charge transfer from absorber to reactive sites. Here, we propose construct directional channels in monolithically integrated electrode, taking carbon dots/carbon nitride (CCN) nanotubes FeOOH/FeCo layered double hydroxide (FFC) nanosheets as representative, boost photoassisted overall water splitting performance. Detailed experimental investigations DFT calculations demonstrate that interfacial C-O-Fe bonds between CCN FFC act channels, facilitating migration photogenerated carriers surfaces. Moreover, situ oxidized Fe/Co species holes trigger lattice oxygen activation, realizing construction Fe-Co dual-site catalytic center efficiently lowering barrier energy for oxidation. As result, CCN@FFC electrode shows multiple functionalities photoelectrocatalysis: only low overpotential 68 mV, 182 1.435 V required deliver 10 mA cm-2 current densities HER, OER, splitting, respectively. This modulation strategy may facilitate design highly active cost-effective multifunctional catalysts conversion storage.

Язык: Английский

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Dual Atom Catalysts for Energy and Environmental Applications

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(40)

Опубликована: Июнь 7, 2023

The pursuit of high metal utilization in heterogeneous catalysis has triggered the burgeoning interest various atomically dispersed catalysts. Our aim this review is to assess key recent findings synthesis, characterization, structure-property relationship and computational studies dual-atom catalysts (DACs), which cover full spectrum applications thermocatalysis, electrocatalysis photocatalysis. In particular, combination qualitative quantitative characterization with cooperation DFT insights, synergies superiorities DACs compare counterparts, high-throughput catalyst exploration screening machine-learning algorithms are highlighted. Undoubtably, it would be wise expect more fascinating developments field as tunable

Язык: Английский

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Detecting and Quantifying Wavelength‐Dependent Electrons Transfer in Heterostructure Catalyst via In Situ Irradiation XPS

Advanced Science, Год журнала: 2022, Номер 10(4)

Опубликована: Ноя. 14, 2022

The identity of charge transfer process at the heterogeneous interface plays an important role in improving stability, activity, and selectivity heterojunction catalysts. And, situ irradiation X-ray photoelectron spectroscopy (XPS) coupled with UV light optical fiber measurement setup is developed to monitor observe between heterojunction. However, in-depth relationship binding energy wavelength missing based on fact that incident formed by coupling different wavelengths. Furthermore, a quantitative understanding numbers remains elusive. Herein, g-C3 N4 /SnO2 model catalyst, wavelength-dependent Boltzmann function describe changes through utilizing continuously adjustable monochromatic XPS technique established. Using this method, study further reveals electrons number can be readily calculated forming asymptotic model. This methodology provides blueprint for deep charge-transfer rules facilitates future development highly active advanced

Язык: Английский

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