Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications

Advanced Science, Год журнала: 2024, Номер 11(33)

Опубликована: Июль 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Язык: Английский

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Toward Practical Li–CO₂ Batteries: Mechanisms, Catalysts, and Perspectives

Accounts of Materials Research, Год журнала: 2024, Номер 5(4), С. 467 - 478

Опубликована: Фев. 28, 2024

ConspectusAchieving the target of carbon neutrality has become a pressing global imperative in world where imminent threat greenhouse gas emissions looms large. Metal–CO2 batteries, which possess dual functions CO2 utilization and electrical energy storage, are considered as one promising emission reduction strategies. Among varieties metal–CO2 Li–CO2 batteries have highest thermodynamic equilibrium potential (∼2.80 V) largest theoretical specific (∼1880 Wh kg–1), making them center research efforts potentially transformational storage technologies. However, development is still its early stages. The complicated evolution mechanisms not been fully understood. Widely accepted products Li2CO3 carbon. These produced following surface-mediated or solution-mediated discharge pathway depending on adsorption cathode catalysts to intermediates solubility electrolytes. During charging, self-decomposition reversible codecomposition could occur while applying different catalysts. In addition selection catalysts, modification electrolyte components control operation conditions can also affect reaction processes, contributing diverse including Li2C2O4, CO, well Li2O Nonetheless, exact determining factors controlling routes inconclusive. Besides, owing intrinsic properties reactants sluggish kinetics at multiphase interfaces, confronted with large overpotentials undesirable parasitic reactions. Further improvement battery performance, especially efficiency cyclic life, necessary propel practical batteries. this Account, we summarize our community's investigation an attractive avenue toward neutrality. We start brief introduction physicochemical in-depth discussion about fundamental reactions across interfaces. Then, pathways underlying affecting involving electrolytes, highlighted. Furthermore, enhancement strategies for from four aspects catalyst design, modification, anode protection, external field assistance presented based recent works. At end provide some directions deepening understanding optimizing broadening their application future carbon-neutral

Язык: Английский

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Regulating nonmetallic species beyond the first coordination shell of single-atom catalysts for high-performance electrocatalysis

Energy & Environmental Science, Год журнала: 2023, Номер 16(9), С. 3679 - 3710

Опубликована: Янв. 1, 2023

Nonmetallic functional species beyond the first coordination shell can affect or even dictate electrocatalytic performance of single-atom catalysts via indirect, long-range interaction with metal atoms.

Язык: Английский

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Constructing Fe‐N₄ Sites through Anion Exchange‐mediated Transformation of Fe Coordination Environments in Hierarchical Carbon Support for Efficient Oxygen Reduction

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(38)

Опубликована: Авг. 4, 2023

Metal single atoms (SAs) anchored in carbon support via coordinating with N are efficient active sites to oxygen reduction reaction (ORR). However, rational design of atom catalysts highly exposed is challenging and urgently desirable. Herein, an anion exchange strategy presented fabricate Fe-N4 moieties hierarchical nanoplates composed hollow spheres (Fe-SA/N-HCS). With the O substituted by atoms, Fe SAs Fe-O4 configuration transformed into ones during thermal activation process. Insights evolution central demonstrate that specific coordination environment can be obtained modulating situ The produces a large quantity electrochemical accessible site high utilization rate . Fe-SA/N-HCS shows excellent ORR electrocatalytic performance half-wave potential 0.91 V (vs. RHE) 0.1 M KOH, outstanding when used rechargeable aqueous flexible Zn-air batteries. pathway for demonstrated this work offers novel SACs various enhanced activity.

Язык: Английский

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CO₂ Conversion Toward Real‐World Applications: Electrocatalysis versus CO₂ Batteries

Advanced Functional Materials, Год журнала: 2023, Номер 33(32)

Опубликована: Апрель 25, 2023

Abstract Electrochemical carbon dioxide (CO 2 ) conversion technologies have become new favorites for addressing environmental and energy issues, especially with direct electrocatalytic reduction of CO (ECO RR) alkali metal‐CO (M–CO batteries as representatives. They are poised to create economic drivers while also paving the way a cleaner more sustainable future humanity. Although still far from practical application, ECO RR has been intensively investigated over last few years, some achievements. In stark contrast, M–CO batteries, aqueous hybrid offer potential combine storage into an integrated system, but their research is in early stages. This article gives insightful review, comparison, analysis recent advances illustrating similarities differences, aiming advance development innovation. Considering crucial role well‐designed functional materials facilitating special attention paid rational design strategies components, such electrodes/catalysts, electrolytes, membranes/separators, at industrial level impact on conversion. Moreover, perspectives suggestions presented facilitate applications.

Язык: Английский

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Insight into Defect Engineering of Atomically Dispersed Iron Electrocatalysts for High‐Performance Proton Exchange Membrane Fuel Cell

Advanced Materials, Год журнала: 2023, Номер 35(46)

Опубликована: Авг. 7, 2023

Abstract Atomically dispersed and nitrogen coordinated iron catalysts (Fe‐NCs) demonstrate potential as alternatives to platinum‐group metal (PGM) in oxygen reduction reaction (ORR). However, the context of practical proton exchange membrane fuel cell (PEMFC) applications, electrode assembly (MEA) performances Fe‐NCs remain unsatisfactory. Herein, improved MEA performance is achieved by tuning local environment Fe‐NC through defect engineering. Zeolitic imidazolate framework (ZIF)‐derived nitrogen‐doped carbon with additional CO 2 activation employed construct atomically sites a controlled number. The species optimal number exhibit excellent ORR high half‐wave 0.83 V 0.5 M H SO 4 . Variation defects allows for fine‐tuning intermediate binding energies changing contribution Fe d‐orbitals, thereby optimizing activity. based on defect‐engineered catalyst found remarkable peak power density 1.1 W cm −2 an /O cell, 0.67 /air rendering it one most active materials at level.

Язык: Английский

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Single‐Atom Mn Catalysts via Integration with Mn Sub Nano‐Clusters Synergistically Enhance Oxygen Reduction Reaction

Small, Год журнала: 2023, Номер 20(22)

Опубликована: Дек. 19, 2023

Integrating single atoms and clusters into one system represents a novel strategy for achieving the desired catalytic performance. In comparison to single-atom catalysts, catalysts combining harness advantages of both, thus displaying greater potential. Nevertheless, constructing single-atom-cluster systems remains challenging, fundamental mechanism enhancing activity elusive. this study, directly confined preparation 3D hollow sea urchin-like carbon structure (Mn

Язык: Английский

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Theoretical research on efficient electrocatalysis of CO2 reduction reaction by borophene loaded transition metals

Surfaces and Interfaces, Год журнала: 2024, Номер 49, С. 104454 - 104454

Опубликована: Май 9, 2024

Язык: Английский

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A molecular view of single-atom catalysis toward carbon dioxide conversion

Chemical Science, Год журнала: 2024, Номер 15(13), С. 4631 - 4708

Опубликована: Янв. 1, 2024

We present critical advances in single-atom catalysis toward CO 2 transformation and address crucial issues about SACs from a molecular point of view.

Язык: Английский

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Microenvironment Engineering of Heterogeneous Catalysts for Liquid-Phase Environmental Catalysis

Chemical Reviews, Год журнала: 2024, Номер 124(20), С. 11348 - 11434

Опубликована: Окт. 9, 2024

Environmental catalysis has emerged as a scientific frontier in mitigating water pollution and advancing circular chemistry reaction microenvironment significantly influences the catalytic performance efficiency. This review delves into engineering within liquid-phase environmental catalysis, categorizing microenvironments four scales: atom/molecule-level modulation, nano/microscale-confined structures, interface surface regulation, external field effects. Each category is analyzed for its unique characteristics merits, emphasizing potential to enhance efficiency selectivity. Following this overview, we introduced recent advancements advanced material system design promote (e.g., purification, transformation value-added products, green synthesis), leveraging state-of-the-art technologies. These discussions showcase was applied different reactions fine-tune regimes improve from both thermodynamics kinetics perspectives. Lastly, discussed challenges future directions engineering. underscores of intelligent materials drive development more effective sustainable solutions decontamination.

Язык: Английский

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