Phase Engineering and Synchrotron-Based Study on Two-Dimensional Energy Nanomaterials

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(17), P. 10750 - 10807

Published: Aug. 15, 2023

In recent years, there has been significant interest in the development of two-dimensional (2D) nanomaterials with unique physicochemical properties for various energy applications. These are often derived from phase structures established through a range physical and chemical design strategies. A concrete analysis real reaction mechanisms 2D requires advanced characterization methods that offer valuable information as much possible. Here, we present comprehensive review on engineering typical focus synchrotron radiation characterizations. particular, intrinsic defects, atomic doping, intercalation, heterogeneous interfaces introduced, together their applications energy-related fields. Among them, synchrotron-based multiple spectroscopic techniques emphasized to reveal phases structures. More importantly, situ employed provide deep insights into structural evolutions under working conditions or processes nanomaterials. Finally, conclusions research perspectives future outlook further light sources integrated discussed.

Language: Английский

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Boosting the Catalytic Activity of Nitrogen Sites by Spin Polarization Engineering for Oxygen Reduction and Wide‐Temperature Ranged Quasi‐Solid Zn–Air Batteries

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 14(4)

Published: Dec. 3, 2023

Abstract The oxygen reduction reaction (ORR) is a crucial cathode for developing quasi‐solid zinc–air batteries (QZABs) with high energy density. However, the activity and stability of catalysts under extreme conditions have not been fully explore. Herein, series systematic experiments theoretical calculations conducted to investigate potential introducing Fe x Co y into nitrogen (N)‐doped porous carbon (NPC) via one‐step pyrolysis form core–shell structure that can effectively enhance catalysts, particularly at low temperatures. Due difference in work function 5.12, 5.11, 5.06 eV, spin‐polarized charge transferred pyridinic‐N site on surface transfer. Consequently, exhibits varying degrees magnetic moment 0.024 µ B , which forming OOH* enhances ORR activity. 5 @NPC catalyst evaluated QZABs −40 °C achieved power density up 117.6 mW cm −2 only 18.7% lower than normal temperature, cycle life 300 h. This study provides means realize design environments explore their application potential.

Language: Английский

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Advances in regulating the electron spin effect toward electrocatalysis applications

eScience, Journal Year: 2024, Volume and Issue: unknown, P. 100264 - 100264

Published: March 1, 2024

Building highly reactive electrocatalysts is of great significance for addressing the energy crisis and developing green energy. Electrocatalytic reactions occur at interface catalysts, where physicochemical properties catalyst surface play a dominant role. In particular, electron spin behavior on has decisive impact catalytic reaction process. This review initially introduces definition methods manipulation. Furthermore, we summarize advanced characterization spin. Then, latest research advancements effect in oxygen reduction reaction, evolution carbon dioxide nitrogen reaction. The mechanisms manipulation these four are thoroughly discussed. Finally, propose key directions future development effects field electrocatalysis. contributes to deeper understanding micromechanisms electrocatalytic reactions.

Language: Английский

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Chemomechanics Engineering Promotes the Catalytic Activity of Spinel Oxides for Sulfur Redox Reaction

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: May 13, 2024

Abstract Cooperative catalysis is a promising approach to enhance the sluggish redox kinetics of lithium polysulfides (LiPSs) for practical lithium–sulfur (Li–S) batteries. However, elusory synergistic effect among multiple active sites makes it challenging accurately customize electronic structure catalysts. Herein, strategy precisely tailoring e g orbitals spinel oxides through chemomechanics engineering porposed regulate LiPSs retention and catalysis. By manipulating regulable cations in Mn x Co 3‐ O 4 , theoretically experimentally revealed that lattice strain induced by Jahn–Teller high‐spin 3+ at octahedral (Oh) can increase occupancy low‐spin Oh which effectively regulates chemical affinity toward establishes an unblocked channel intrinsic charge transfer. This leads volcano‐type correlation between sulfur activity. Benefitting from cooperative dual‐active sites, MnCo 2 with average 0.45 affords most appropriate adsorption strength rapid LiPSs, leading remarkable rate performance capacity assembled Li–S work demonstrates promise optimizing achieve efficient

Language: Английский

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Diatomic Iron with a Pseudo-Phthalocyanine Coordination Environment for Highly Efficient Oxygen Reduction over 150,000 Cycles

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(36), P. 24842 - 24854

Published: Aug. 26, 2024

Atomically dispersed Fe-N-C catalysts emerged as promising alternatives to commercial Pt/C for the oxygen reduction reaction. However, majority of showed unsatisfactory activity and durability due their inferior O-O bond-breaking capability rapid Fe demetallization. Herein, we create a pseudo-phthalocyanine environment coordinated diatomic iron (Fe

Language: Английский

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Progress in manipulating spin polarization for solar hydrogen production

Materials Reports Energy, Journal Year: 2024, Volume and Issue: 4(1), P. 100253 - 100253

Published: Jan. 23, 2024

Photocatalytic and photoelectrochemical water splitting using semiconductor materials are effective approaches for converting solar energy into hydrogen fuel. In the past few years, a series of photocatalysts/photoelectrocatalysts have been developed optimized to achieve efficient production. Among various optimization strategies, regulation spin polarization can tailor intrinsic optoelectronic properties retarding charge recombination enhancing surface reactions, thus improving solar-to-hydrogen (STH) efficiency. This review presents recent advances in enhance polarized-dependent evolution activity. Specifically, manipulation strategies several typical (e.g., metallic oxides, sulfides, non-metallic semiconductors, ferroelectric materials, chiral molecules) described. end, critical challenges perspectives towards future conversion briefly provided.

Language: Английский

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Realizing the 4e^–/2e^– Pathway Transition of O₂ Reduction on Co–N₄–C Catalysts by Regulating the Chemical Structures beyond the Second Coordination Shells

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(8), P. 5961 - 5971

Published: April 4, 2024

The catalytic performance of single-atom catalysts (SACs) is vitally determined by their coordination environments. So far, the manipulation SACs has been mainly focused on first and second nearest structures center atoms. We herein demonstrate that chemical environments beyond shells also significantly influence behaviors SACs. Our findings reveal presence graphitic nitrogen can induce a shift O2 reduction pathway CoN4C sites from an energy-conversion favorite 4e– to H2O2-production desirable 2e– pathway. remote N tunes electronic structure Co lower-spin state higher-spin state, as proved zero-field cooling (ZFC) temperature-dependent magnetic susceptibility, which weakens adsorption O2/*OOH, ultimately enhancing selectivity toward H2O2. It further revealed may be universally present in other such FeN4C MnN4C. Impressively, N-doped exhibits high H2O2 Faraday efficiency (82%) flow cell, with remarkable yield 0.096 mmol cm–2 h–1 for 200 h at 0.358 V (vs RHE), sufficient many applications electro-Fenton-like degradation malachite green demonstrated feasibility electrosynthesis.

Language: Английский

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Spin‐Regulated Fenton‐Like Catalysis for Nonradical Oxidation over Metal Oxide@Carbon Composites

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(36)

Published: April 24, 2024

Abstract The spin state of the transition metal species (TMs) has been recognized as a critical descriptor in Fenton‐like catalysis. raised dispersed TMs carbon will enhance redox processes with adsorbed peroxides and improve oxidation performance. Nevertheless, establishing spin‐activity correlations for encapsulated TM nanoparticles remains challenging because difficulties fine‐tuning insufficient understanding orbital hybridization states upon interaction peroxides. Here, advantage fast‐temperature heating/quenching microwave thermal shock is taken to engineer structure within N‐doped graphitic carbons. reduced particle size enhanced TMs‐carbon coupling increase surface entropy regulate e g electron filling high‐spin TM‐N coordination, endowing electrons high mobility facilitating peroxymonosulfate (PMS) adsorption. strong interactions further uplift PMS O 2p band position toward Fermi level thus elevate potential surface‐activated (PMS * ) dominant nonradical pollutant degradation. deciphered hybridizations engineered enlighten smart design spin‐regulated nanocomposites advanced water purification.

Language: Английский

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Prussian Blue Analogues and Their Derivatives: From Elaborate Microstructure Design to Boosted Fenton-Like Application

Accounts of Materials Research, Journal Year: 2024, Volume and Issue: 5(5), P. 585 - 599

Published: April 9, 2024

ConspectusHeterogeneous Fenton-like reaction is a promising process for refractory wastewater treatment. Among the various heterogeneous catalysts, Prussian blue (PB) and analogues (PBAs) show great potential hydrogen peroxide persulfate activation owing to their low toxicity, simple preparation, high activity. To further improve catalytic activity of PBAs derivatives (PBDs), many efforts have been made overcome instability crystal structure develop feasible methodologies prepare PBAs/PBDs with diverse morphologies compositions. In this Account, our recent achievements on novel synthetic strategies obtain controlled morphologies, geometric sites, electronic structures were systematically summarized. The physicochemical properties contribution in advanced oxidation processes (AOPs) also discussed.First, we focus developing synthesis technology (such as "copolymer-co-morphology" conception) controllable morphology. By regulating chelating agents, surfactants, metal ions, preparation conditions constructing heterojunction, stability was significantly improved during redox reaction. Notably, inherit characteristics PBAs, topological transformation strategy applied fabricate oxides similar those through thermal calcination under an aerobic atmosphere. Subsequently, has extensively single-atom nitrides, zerovalent metals via treatment inert/reducing atmospheres. These provide guidance devising materials superior cycling tests not only reactions but other systems. addition property optimization, relationship between deliberately designed first explored depth using 57Fe Mössbauer spectroscopy. Moreover, benefiting from these efficient techniques conscientious explorations, research elucidated important descriptors intrinsic pathways revealed significant effect external energy (ultraviolet visible light) PBAs/PBDs-dominant findings inspiration application additional energy. Finally, challenges development prospects AOPs are comprehensively discussed. Overall, Account provides comprehensive insights into fabrication strategies, properties, local structures, correlation mechanisms analysis paves way future catalysis fields.

Language: Английский

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Magnetic Measurements Applied to Energy Storage

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(24)

Published: April 29, 2023

Abstract How to increase energy storage capability is one of the fundamental questions, it requires a deep understanding electronic structure, redox processes, and structural evolution electrode materials. These thorny problems now usually involve spin–orbit, spin‐related electron configuration, etc., which cannot be probed using conventional testing techniques. Considering intimate connection between spin magnetic properties, as probe, measurements make possible analyze processes from perspective magnetism. Owing characterizing properties high compatibility with field, are proven powerful tools for contributing progress storage. In this review, several typical applications in alkali metal ion batteries research emphasize associated electrochemical performance materials, presented. Finally, current challenges prospects enhanced analysis systems discussed.

Language: Английский

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