Embedding Atomically Dispersed Iron Sites in Nitrogen‐Doped Carbon Frameworks‐Wrapped Silicon Suboxide for Superior Lithium Storage

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

Опубликована: Дек. 5, 2022

Abstract Silicon suboxide (SiO x ) has attracted widespread interest as Li‐ion battery (LIB) anodes. However, its undesirable electronic conductivity and apparent volume effect during cycling impede practical applications. Herein, sustainable rice husks (RHs)‐derived SiO 2 are chosen a feedstock to design /iron–nitrogen co‐doped carbon (Fe–N–C) materials. Using facile electrospray‐carbonization strategy, nanoparticles (NPs) encapsulated in the nitrogen‐doped (N–C) frameworks decorating atomically dispersed iron sites. Systematic characterizations including high‐angle annular dark‐field scanning transmission electron microscopy (HAADF‐STEM) X‐ray absorption fine structure (XAFS) verify existence of Fe single atoms typical coordination environment. Benefiting from structural compositional merits, /Fe–N–C anode delivers significantly improved discharge capacity 799.1 mAh g −1 , rate capability, exceptional durability, compared with pure /N–C, which been revealed by density functional theory (DFT) calculations. Additionally, electrochemical tests situ diffraction (XRD) analysis reveal oxidation Li Si phase storage mechanism. The synthetic strategy is universal for synthesis metal atoms/clusters N–C NPs. Meanwhile, this work provides impressive insights into developing various LIB materials suffering inferior huge fluctuations.

Язык: Английский

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Space‐Confined Metal Ion Strategy for Carbon Materials Derived from Cobalt Benzimidazole Frameworks with High Desalination Performance in Simulated Seawater

Advanced Materials, Год журнала: 2023, Номер 35(23)

Опубликована: Март 29, 2023

Various metal ions with different valence states (Mg2+ , Al3+ Ca2+ Ti4+ Mn2+ Fe3+ Ni2+ Zn2+ Pb2+ Ba2+ Ce4+ ) are successfully confined in quasi-microcube shaped cobalt benzimidazole frameworks using a space-confined synthesis strategy. More importantly, series of derived carbon materials that confine obtained by high-temperature pyrolysis. Interestingly, the exhibited electric double-layer and pseudocapacitance properties because presence various states. Moreover, additional within may create new phases, which can accelerate Na+ insertion/extraction thus increase electrochemical adsorption. Density functional theory results showed Ti exhibit enhanced resulting from characteristic anatase crystalline phases TiO2 . The Ti-containing have an impressive desalination capacity (62.8 mg g-1 capacitive deionization (CDI) applications high cycling stability. This work provides facile synthetic strategy for confinement metal-organic supports further development seawater CDI.

Язык: Английский

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Conductive MOFs for electrocatalysis and electrochemical sensor

eScience, Год журнала: 2023, Номер 3(6), С. 100133 - 100133

Опубликована: Апрель 11, 2023

Two-dimensional conductive metal–organic frameworks (2D-cMOFs) are a class of 2D layered MOFs with excellent electrical conductivity and other electronic properties. In recent years, their porous structure dense active sites have been widely used in electrocatalysis electrochemical sensing. The large electron delocalization domains generated by an extended π-conjugated framework through the covalent bonding between metal organic ligand endow them unique high conductivity. Yet despite few promising applications, current research rarely addresses “structure–property relationship.” This review discusses rational design 2D-cMOFs extraordinary performance. We introduce several representative describe focusing on catalysis small molecule detection. By correlating performance materials these applications corresponding mechanisms, we aim to uncover key structural features that lead engineered properties functions.

Язык: Английский

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Enhanced Active Sites and Stability in Nano‐MOFs for Electrochemical Energy Storage through Dual Regulation by Tannic Acid

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(41)

Опубликована: Авг. 21, 2023

The limited active sites and poor acid-alkaline solution stability of metal-organic frameworks (MOFs), significantly limit their wider application. In this study, the acid property tannic (TA) was used as an etchant to etch surface-active sites. Subsequently, further chelation protonated TA with exposed metal site can effectively protect ions. Meanwhile, provided a large amount phenolic hydroxyl groups, which greatly improve imidazolate-coordinated MOFs. electrochemical test results indicated that MOFs composite materials synthesized using scheme had high specific capacitance stability. And mechanism its reaction process explored through in situ X-ray diffraction (XRD) theoretical calculations. addition, same treatment carried out series carboxyl-coordinated MOFs, confirmed principle obtain higher This paper explains functionalization nano-MOFs by polyphenolic compounds, providing new ideas for research nano-MOFs.

Язык: Английский

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Single Cu–N₄sites enable atomic Fe clusters with high-performance oxygen reduction reactions

Energy & Environmental Science, Год журнала: 2023, Номер 16(8), С. 3576 - 3586

Опубликована: Янв. 1, 2023

Atomic Fe clusters functionalized by Cu–N 4 sites with enhanced oxygen reduction reactions (ORRs) in alkaline and acidic media.

Язык: Английский

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Regulating Intramolecular Electron Transfer of Nickel‐Based Coordinations through Ligand Engineering for Aqueous Batteries

Advanced Materials, Год журнала: 2023, Номер 35(48)

Опубликована: Сен. 25, 2023

The integration of electronic effects into complexes for the construction novel materials has not yet attracted significant attention in field energy storage. In current study, eight one-dimensional (1D) nickel-based salicylic acid (Ni-XSAs, X = pH, pMe, pMeO, mMe, pBr, pCl, pF, and pCF3 ), are prepared by ligand engineering. coordination environments Ni-XSAs explored using X-ray absorption fine structure spectroscopy. charge transfer is modulated according to difference electron-donating ability substituents, combination with frontier orbital theory. Furthermore, density functional theory used investigate effect substituent position on properties complexes. Ni-mMeSA exhibits better electrical conductivity than Ni-pMeSA. electrochemical performance as an aqueous battery cathode remarkably improved a maximum 0.30 mWh cm-2 (125 Wh kg-1 ) peak power 33.72 mW (14.03 kW ). This study provides ideas application new chemistry science.

Язык: Английский

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Pyridine‐Regulated Lamellar Nickel‐Based Metal–Organic Framework (Ni‐MOF) for Nonenzymatic Electrochemical Glucose Sensor

Advanced Science, Год журнала: 2023, Номер 10(27)

Опубликована: Июль 20, 2023

2D metal-organic frameworks (MOFs) are considered as promising electrochemical sensing materials and have attracted a lot of attention in recent years. Compared with bulk MOFs, the construction MOFs can increase exposure active sites by obtaining larger surface area ratio. Herein, facile one-pot hydrothermal synthesis pyridine-regulated lamellar Ni-MOFs ultrathin well-defined morphology is described. structure, Ni-MOF has higher site density, showing better glucose performance. The exhibits fast amperometric response less than 3 s high sensitivity 907.54 µA mm-1 cm-2 toward wide linear range 0.5-2665.5 µm. Furthermore, also possesses excellent stability reproducibility, be used to detect accuracy reliability different environments.

Язык: Английский

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Confining Iodine into Metal‐Organic Framework Derived Metal‐Nitrogen‐Carbon for Long‐Life Aqueous Zinc‐Iodine Batteries

Advanced Materials, Год журнала: 2024, Номер 36(38)

Опубликована: Июль 31, 2024

Abstract Aqueous zinc–iodine batteries (AZIBs) are highly appealing for energy requirements owing to their safety, cost‐effectiveness, and scalability. However, the inadequate redox kinetics severe shuttling effect of polyiodide ions impede commercial viability. Herein, several Zn‐MOF‐derived porous carbon materials designed, further preparation iron–doped (Fe–N–C, M9) with varied Fe doping contents is optimized based on a facile self‐assembly/carbonization approach. M9, atomic coordinated nitrogen atoms, employed as an efficient cathode host AZIBs. Functional modifications hosts involving species levels investigated. The adsorption tests, in situ Raman spectroscopy, UV–vis results demonstrate capability charge‐discharge mechanism iodine species. Furthermore, experimental findings theoretical analyses have proven that conversion enhanced through physicochemical confinement effect. This study offers basic principles strategic design single‐atom dispersed high‐performance Flexible soft–pack battery wearable microbattery applications also implications future long‐life aqueous designs.

Язык: Английский

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Harnessing the power of functionalized biochar: progress, challenges, and future perspectives in energy, water treatment, and environmental sustainability

Biochar, Год журнала: 2024, Номер 6(1)

Опубликована: Март 14, 2024

Abstract The swift advancement of sustainable energy technologies, coupled with the urgent need to address environmental challenges, has generated considerable interest in multifaceted applications biochar materials promote energy, water, and sustainability. This comprehensive review examines recent advancements production functionalized materials, emphasizing their pivotal roles conversion storage, wastewater treatment, CO 2 reduction, soil amelioration, promotion carbon neutrality within a circular economy framework. functionalization involves surface chemistry porosity modifications, achieved through techniques like templating, chemical activation, metal impregnation, or heteroatom doping. These modifications substantially enhance catalytic activity, storage capacity, cycling stability making them particularly effective diverse such as water splitting, fuel cells, supercapacitors. Additionally, demonstrate remarkable efficacy catalysts adsorbents proficiently removing pollutants heavy metals, organic contaminants, nutrients, thereby facilitating resource recovery from wastewater. also underscores potential capture conversion, exploring innovative strategies augment adsorption capacity state-of-the-art processes for transforming captured into valuable fuels chemicals. In summary, this offers insights research, underscoring its substantial commercial versatile material contributing cleaner more future. Article Highlights current status research is comprehensively reviewed. fields critically examined. Technology readiness levels (TRLs) various biochar-based technologies are evaluated. Graphical

Язык: Английский

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Design and Functionalization of Lignocellulose‐Derived Silicon‐Carbon Composites for Rechargeable Batteries

Advanced Energy Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 30, 2024

Abstract Silicon/carbon (Si/C) composites present great potential as anode materials for rechargeable batteries since the integrate high specific capacity and preferable cycling stability from Si C components, respectively. Functional Si/C based on lignocellulose have attracted wide attention due to advantages lignocellulose, including sustainability property, flexible structural tunability, diverse physicochemical functionality. Although flourishing development of boosts studies lignocellulose‐derived with electrochemical performance, publications that comprehensively clarify design functionalization these high‐profile are still scarce. Accordingly, this review first systematically summarizes recent advances in after a brief clarification about selection sources self extraneous sources. Afterward, strategies, nanosizing, porosification, magnesiothermic reduction material well heteroatom modification material, specifically highlighted. Besides, applications Si/C‐based elaborated. Finally, discusses challenges prospects application energy storage provides nuanced viewpoint regarding topic.

Язык: Английский

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