TiO₂/FePS₃ S‐Scheme Heterojunction for Greatly Raised Photocatalytic Hydrogen Evolution

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(46)

Published: Oct. 6, 2022

Abstract The aggravating extreme climate changes and natural disasters stimulate the exploration of low‐carbon/zero‐carbon alternatives to traditional carbon‐based fossil fuels. Solar‐to‐hydrogen (STH) transformation is considered as appealing route convert renewable solar energy into carbon‐free hydrogen. Restricted by low efficiency high cost noble metal cocatalysts, high‐performance cost‐effective photocatalysts are required realize realistic STH transformation. Herein, 2D FePS 3 (FPS) nanosheets anchored with TiO 2 nanoparticles (TiO /FePS ) synthesized tested for photocatalytic hydrogen evolution reaction. With integration FPS, H ‐evolution rate on radically increased ≈1686%, much faster than that alone. origin greatly raised activity revealed theoretical calculations various advanced characterizations, such transient‐state photoluminescence spectroscopy/surface photovoltage spectroscopy, in situ atomic force microscopy combined Kelvin probe (AFM‐KPFM), X‐ray photoelectron spectroscopy (XPS), synchrotron‐based absorption near edge structure. Especially, AFM‐KPFM XPS together confirm electron transport pathway light illumination, unveiling efficient separation/transfer charge carrier step‐scheme heterojunction. This work sheds designing fabricating novel material‐based S‐scheme heterojunctions photocatalysis.

Language: Английский

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Catalytic effect in Li-S batteries: From band theory to practical application

Materials Today, Journal Year: 2022, Volume and Issue: 57, P. 84 - 120

Published: June 9, 2022

Language: Английский

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Flexible Zinc–Air Batteries with Ampere‐Hour Capacities and Wide‐Temperature Adaptabilities

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(13)

Published: Jan. 30, 2023

Flexible Zn-air batteries (FZABs) have significant potentials as efficient energy storage devices for wearable electronics because of their safeties and high energy-to-cost ratios. However, application is limited by short cycle lives, low discharge capacities per cycle, charge/discharge polarizations. Accordingly, herein, a poly(sodium acrylate)-polyvinyl alcohol (PANa-PVA)-ionic liquid (IL) hydrogel (PANa-PVA-IL) prepared using hygroscopic IL, 1-ethyl-3-methylimidazolium chloride, an additive twin-chain PANa-PVA. PANa-PVA-IL exhibits conductivity 306.9 mS cm-1 water uptake 2515 wt% at room temperature. Moreover, low-cost bifunctional catalyst, namely, Co9 S8 nanoparticles anchored on N- S-co-doped activated carbon black pearls 2000 (Co9 -NSABP), synthesized, which demonstrates O2 reversibility potential gap 0.629 V. FZABs based -NSABP demonstrate 1.67 mAh cm-2 long lives 330 h. Large-scale flexible rechargeable pouch cells exhibit total 1.03 Ah densities 246 Wh kgcell-1 . This study provides new information about hydrogels with ionic conductivities uptakes should facilitate the in electronics.

Language: Английский

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Vacancy Defects in 2D Transition Metal Dichalcogenide Electrocatalysts: From Aggregated to Atomic Configuration

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(50)

Published: Oct. 3, 2022

Abstract Vacancy defect engineering has been well leveraged to flexibly shape comprehensive physicochemical properties of diverse catalysts. In particular, growing research effort devoted chalcogen anionic vacancies (S/Se/Te) 2D transition metal dichalcogenides (2D TMDs) toward the ultimate performance limit electrocatalytic hydrogen evolution reaction (HER). spite remarkable progress achieved in past decade, systematic and in‐depth insights into state‐of‐the‐art vacancy for 2D‐TMDs‐based electrocatalysis are still lacking. Herein, this review delivers a full picture evolving from aggregated atomic configurations covering their development background, controllable manufacturing, thorough characterization, representative HER application. Of particular interest, deep‐seated correlations between specific regulation routes resulting catalytic improvement logically clarified terms rearrangement, charge redistribution, energy band variation, intermediate adsorption–desorption optimization, charge/mass transfer facilitation. Beyond that, broader vision is cast cutting‐edge fields vacancy‐engineering‐based single‐atom catalysis dynamic structure–performance across catalyst service lifetime. Together with critical discussion on residual challenges future prospects, sheds new light rational design advanced catalysts navigates application high‐efficiency conversion storage fields.

Language: Английский

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Identifying the Role of Lewis‐base Sites for the Chemistry in Lithium‐Oxygen Batteries

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(32)

Published: June 10, 2023

Abstract Lewis‐base sites have been widely applied to regulate the properties of Lewis‐acid in electrocatalysts for achieving a drastic technological leap lithium‐oxygen batteries (LOBs). Whereas, direct role and underlying mechanism chemistry LOBs are still rarely elucidated. Herein, we comprehensively shed light on pivotal promoting electrocatalytic reaction processes by constructing metal–organic framework containing (named as UIO‐66‐NH 2 ). The density functional theory (DFT) calculations demonstrate can act electron donors that boost activation O /Li during discharged‐charged process, resulting accelerated kinetics LOBs. More importantly, situ Fourier transform infrared spectra DFT firstly convert Li growth from surface‐adsorption solvation‐mediated due capture + upon discharged which weakens adsorption energy towards LiO . As proof concept, LOB based achieve high discharge specific capacity (12 661 mAh g −1 ), low overpotential (0.87 V) long cycling life (169 cycles). This work reveals sites, guide design featuring Lewis‐acid/base dual centers

Language: Английский

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MXene Analogue: A 2D Nitridene Solid Solution for High‐Rate Hydrogen Production

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(27)

Published: April 19, 2022

Electrocatalysts for high-rate hydrogen evolution reaction (HER) are crucial to clean fuel production. Nitrogen-rich 2D transition metal nitride, designated "nitridene", has shown promising HER performance because of its unique physical/chemical properties. However, synthesis is hindered by the sluggish growth kinetics. Here first time using a catalytic molten-salt method, we facilely synthesized V-Mo bimetallic nitridene solid solution, V0.2 Mo0.8 N1.2 , with tunable electrocatalytic property. The reduces barrier and facilitates V dissolution via monomer assembly, as confirmed synchrotron spectroscopy ex situ electron microscopy. Furthermore, merging computational simulations, confirm that doping leads an optimized electronic structure fast protons coupling produce hydrogen. These findings offer quantitative engineering strategy developing analogues MXenes energy conversions.

Language: Английский

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Recent progress of transition metal-based catalysts as cathodes in O₂/H₂O-involved and pure Li–CO₂batteries

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(3), P. 792 - 829

Published: Jan. 1, 2023

The composition, structure, reaction mechanism of transition metal-based catalysts and their effects on the electrochemical performance Li-CO 2 cells were summarized, some perspectives for development put forward.

Language: Английский

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All-Solid-State Photo-Assisted Li-CO₂ Battery Working at an Ultra-Wide Operation Temperature

ACS Nano, Journal Year: 2022, Volume and Issue: 16(8), P. 12364 - 12376

Published: Aug. 1, 2022

At present, photoassisted Li-air batteries are considered to be an effective approach overcome the sluggish reaction kinetics of batteries. And, organic liquid electrolyte is generally adopted by current conventional However, superior catalytic activity cathode would in turn fasten degradation electrolyte, leading limited battery cycling life. Herein, we tame above limitation traditional system for Li-CO2 constructing a all-solid-state with integrated bilayer Au@TiO2/Li1.5Al0.5Ge1.5(PO4)3 (LAGP)/LAGP (ATLL) framework, which can essentially improve stability. Taking advantage photoelectric and photothermal effects, Au@TiO2/LAGP layer enables acceleration slow carbon dioxide reduction evolution processes. The LAGP could resolve problem decomposition under illumination. double-layer framework endows direct transportation heat Li+ entire system. achieves ultralow polarization 0.25 V illumination, as well high round-trip efficiency 92.4%. Even at extremely low temperature -73 °C, still deliver small 0.6 converting solar energy into achieve self-heating. This study not but also applied other systems, constituting significant step toward practical application

Language: Английский

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Structure modulation of two-dimensional transition metal chalcogenides: recent advances in methodology, mechanism and applications

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(4), P. 1215 - 1272

Published: Jan. 1, 2023

Together with the development of two-dimensional (2D) materials, transition metal dichalcogenides (TMDs) have become one most popular series model materials for fundamental sciences and practical applications. Due to ever-growing requirements customization multi-function, dozens modulated structures been introduced in TMDs. In this review, we present a systematic comprehensive overview structure modulation TMDs, including point, linear out-of-plane structures, following updating conventional classification silicon related bulk semiconductors. particular, focus on structural characteristics TMD analyse corresponding root causes. We also summarize recent progress modulating methods, mechanisms, properties applications based structures. Finally, demonstrate challenges prospects TMDs forecast potential directions about what how breakthroughs can be achieved.

Language: Английский

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Interfacial engineering of transition metal dichalcogenide/carbon heterostructures for electrochemical energy applications

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(22), P. 7802 - 7847

Published: Jan. 1, 2023

This review provides a fundamental understanding of three types interfacial engineering in TMDC/C heterostructures and guidance for designing electrochemical energy applications.

Language: Английский

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