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Pore space partition of metal-organic frameworks for gas storage and separation 储气分离用金属-有机骨架的孔隙空间划分
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-07-01 Epub Date: 2022-06-30 DOI: 10.1016/j.enchem.2022.100080
Anh N. Hong , Huajun Yang , Xianhui Bu , Pingyun Feng

Pore space partition (PSP) concept is a synthetic design concept and can also serve as a structure analysis method useful for next-step synthetic planning and execution. PSP provides an integrated chemistry-topology-focused tool to design new materials platforms. While PSP is no less effective for making large-pore materials, the growing importance of small-molecule gas storage and separation for green-energy applications provides impetus for developing small-pore materials for which the PSP strategy is uniquely suited. Currently, the best embodiment of the PSP concept is the partitioned-acs (pacs) platform in which both fine or coarse adjustments to the building blocks have sparked a transformation of a prototype framework into a huge and continuously expanding family of chemically robust materials with controllable pore metrics and functionalities suitable for tailored applications. The pacs compositional diversity results from the platform's intrinsic multi-module nature, geometric flexibility and tolerance towards individual module variations, and mutual structure-directing effects among various modules, all of which combine to enable the molecular-level uniform co-assemblies of chemical components rarely seen together elsewhere. In this contribution, we present an overview of different pore space engineering methods and how different MOF materials have contributed to important advances in chemical stability, industrial gas storage and gas separation. In particular, we will focus on synthetic assembly of the pacs system, highlighting the differences of pacs materials from other MOF platforms and advantages of pacs materials in enhancing various MOF properties.

孔隙空间划分(PSP)概念是一种综合设计概念,也可以作为一种结构分析方法,对下一步的综合规划和执行有用。PSP提供了一个集成的化学拓扑工具来设计新的材料平台。虽然PSP在制造大孔材料方面同样有效,但小分子气体储存和分离在绿色能源应用中的重要性日益增加,这为开发小孔材料提供了动力,而PSP策略是唯一适合的。目前,PSP概念的最佳体现是分区acs (pacs)平台,在该平台中,对构建块进行精细或粗略的调整,引发了原型框架向巨大且不断扩展的化学坚固材料家族的转变,这些材料具有可控制的孔隙指标和适合定制应用的功能。pacs的成分多样性源于平台固有的多模块特性、几何灵活性和对单个模块变化的容忍度,以及各个模块之间的相互结构导向效应,所有这些因素结合在一起,使化学成分在分子水平上均匀地协同组装在一起,在其他地方很少见到。在这篇文章中,我们概述了不同的孔隙空间工程方法,以及不同的MOF材料如何在化学稳定性、工业气体储存和气体分离方面取得重要进展。我们将特别关注pacs系统的合成组装,突出pacs材料与其他MOF平台的区别,以及pacs材料在提高各种MOF性能方面的优势。
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引用次数: 24
Advanced porous organic polymer membranes: Design, fabrication, and energy-saving applications 先进的多孔有机聚合物膜:设计、制造和节能应用
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-07-01 Epub Date: 2022-06-28 DOI: 10.1016/j.enchem.2022.100079
Yanpei Song, Changjia Zhu, Shengqian Ma

Membrane separation technology is of great research interest in industry owing to its unparalleled merits such as high selectivity with unsuppressed permeability, reduced carbon footprint, small capital investment, and low energy consumption in comparison to traditional separation techniques. In the last few decades, polyamide membranes dominate the membrane industry until the porous organic polymers (POPs) get a ticket into the area of membrane separation. POPs bearing rich pore architectures and feasible functionalization are ready for fabricating novel membranes for rapid and precise molecular sieving. Here, a background overview of separation technology is provided, followed by a brief introduction of various POP-based membranes and the fabrication approaches of these membranes. Then, recent advancements of POP-bases membranes in energy-saving applications including gas separation and liquid separation are highlighted together with discussions about membrane design and generation involved. Finally, a concise conclusion with our perspective and challenges remaining for the future development of POP-based membranes are outlined.

膜分离技术与传统分离技术相比,具有选择性高、渗透性不受抑制、碳足迹少、投资少、能耗低等优点,受到工业领域的广泛关注。在过去的几十年里,聚酰胺膜一直主导着膜工业,直到多孔有机聚合物(pop)进入膜分离领域。具有丰富的孔结构和可行的功能化的持久性有机污染物已经准备好制造用于快速和精确分子筛选的新型膜。本文对分离技术的背景进行了概述,然后简要介绍了各种基于pop的膜和这些膜的制备方法。然后,重点介绍了pop基膜在气体分离和液体分离等节能应用方面的最新进展,并对膜的设计和生产进行了讨论。最后,简要总结了我们对pop基膜未来发展的展望和面临的挑战。
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引用次数: 12
Application of MOFs and COFs for photocatalysis in CO2 reduction, H2 generation, and environmental treatment mof和COFs光催化在CO2还原、H2生成和环境处理中的应用
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-07-01 Epub Date: 2022-06-25 DOI: 10.1016/j.enchem.2022.100078
Yifeng Zhang , Hangxi Liu , Feixue Gao , Xiaoli Tan , Yawen Cai , Baowei Hu , Qifei Huang , Ming Fang , Xiangke Wang

Photocatalysis has been widely studied because it can use inexhaustible solar energy as an energy source while solving the problems of fossil fuel depletion and environmental pollution facing the 21st century. Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs), with many advantages such as high physical/chemical stability, tunable bandgap, structural diversity, large specific surface area, etc., are considered important propellants for building better photocatalytic platforms and achieving breakthroughs. This review outlines the applications of MOFs and COFs for photocatalysis in CO2 reduction, H2 generation, and environmental pollution treatment, and elucidates the relevant photocatalytic mechanisms. In particular, the methods and mechanisms for improving the photocatalytic performance of MOFs and COFs are summarized and discussed from the three aspects. Finally, the current limitations, challenges, perspectives and future development opportunities of COFs/MOFs and COF-/MOF-based photocatalysts are summarized and prospected.

光催化由于可以利用取之不尽的太阳能作为能源,同时解决21世纪面临的化石燃料枯竭和环境污染问题而受到广泛的研究。金属有机骨架(MOFs)和共价有机骨架(COFs)具有物理/化学稳定性高、带隙可调、结构多样性大、比表面积大等优点,被认为是构建更好的光催化平台和实现突破的重要推进剂。本文综述了mof和COFs光催化在CO2还原、H2生成和环境污染处理等方面的应用,并对其光催化机理进行了阐述。特别从三个方面对提高mof和COFs光催化性能的方法和机理进行了总结和讨论。最后,对目前COFs/ mof及COF-/ mof基光催化剂的局限性、挑战、发展前景和未来发展机遇进行了总结和展望。
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引用次数: 211
Impact of urbanisation and environmental factors on spatial distribution of COVID-19 cases during the early phase of epidemic in Singapore. 城市化和环境因素对新加坡疫情早期COVID-19病例空间分布的影响
IF 3.8 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-06-13 DOI: 10.1038/s41598-022-12941-8
Murali Krishna Gurram, Min Xian Wang, Yi-Chen Wang, Junxiong Pang

Geographical weighted regression (GWR) can be used to explore the COVID-19 transmission pattern between cases. This study aimed to explore the influence from environmental and urbanisation factors, and the spatial relationship between epidemiologically-linked, unlinked and imported cases during the early phase of the epidemic in Singapore. Spatial relationships were evaluated with GWR modelling. Community COVID-19 cases with residential location reported from 21st January 2020 till 17th March 2020 were considered for analyses. Temperature, relative humidity, population density and urbanisation are the variables used as exploratory variables for analysis. ArcGIS was used to process the data and perform geospatial analyses. During the early phase of COVID-19 epidemic in Singapore, significant but weak correlation of temperature with COVID-19 incidence (significance 0.5-1.5) was observed in several sub-zones of Singapore. Correlations between humidity and incidence could not be established. Across sub-zones, high residential population density and high levels of urbanisation were associated with COVID-19 incidence. The incidence of COVID-19 case types (linked, unlinked and imported) within sub-zones varied differently, especially those in the western and north-eastern regions of Singapore. Areas with both high residential population density and high levels of urbanisation are potential risk factors for COVID-19 transmission. These findings provide further insights for directing appropriate resources to enhance infection prevention and control strategies to contain COVID-19 transmission.

地理加权回归(GWR)可用于探索病例之间的 COVID-19 传播模式。本研究旨在探讨环境和城市化因素的影响,以及新加坡疫情早期流行病学相关病例、非相关病例和输入病例之间的空间关系。利用 GWR 模型对空间关系进行了评估。分析中考虑了 2020 年 1 月 21 日至 2020 年 3 月 17 日期间报告的居住地社区 COVID-19 病例。温度、相对湿度、人口密度和城市化是分析的探索变量。ArcGIS 用于处理数据和进行地理空间分析。在新加坡 COVID-19 流行的早期阶段,在新加坡的几个分区观察到温度与 COVID-19 发病率之间存在显著但微弱的相关性(显著性为 0.5-1.5)。湿度与发病率之间的相关性无法确定。在各个分区,高居住人口密度和高城市化水平与 COVID-19 的发病率有关。各分区内 COVID-19 病例类型(关联、非关联和输入)的发病率各不相同,尤其是新加坡西部和东北部地区。居住人口密度高和城市化程度高的地区是 COVID-19 传播的潜在风险因素。这些发现提供了进一步的见解,有助于引导适当的资源来加强感染预防和控制策略,以遏制 COVID-19 的传播。
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引用次数: 0
Ionic Liquid Electrolytes for Next-generation Electrochemical Energy Devices 用于新一代电化学能源装置的离子液体电解质
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-05-01 Epub Date: 2022-05-04 DOI: 10.1016/j.enchem.2022.100075
Yayun Zheng , Di Wang , Shubham Kaushik , Shaoning Zhang, Tomoki Wada, Jinkwang Hwang, Kazuhiko Matsumoto, Rika Hagiwara

The development of future energy devices that exhibit high safety, sustainability, and high energy densities to replace the currently dominant lithium-ion batteries has gained significant attention in recent years. Although the various energy devices available have different technological requirements, electrolyte formulation still remains a fundamental element of these state-of-the-art systems. Among the trending electrolyte contenders, ionic liquids, which are entirely comprised of cations and anions, provide a combination of several unique physicochemical and electrochemical properties, and exceptional safety. In this review, the fundamental properties of IL, their progress and milestones, and the directions for their future development and applications in next-generation energy devices are summarized. Each section will comprehensively review the latest progress and technology trends utilizing IL electrolytes focusing on Li-, Na-, K-ion batteries, metal anode batteries, sulfur and oxygen batteries, multivalent metal-ion batteries, and supercapacitors, with early studies mentioned where relevant. The benefits of using ionic liquid electrolytes on each system and pertinent improvements in performance are delineated in comparison to systems utilizing conventional electrolytes. Finally, prospects and challenges associated with the applications of ionic liquid electrolytes to future energy devices are also discussed.

近年来,开发具有高安全性、可持续性和高能量密度的未来能源设备以取代目前占主导地位的锂离子电池已受到广泛关注。尽管各种能源装置有不同的技术要求,电解质配方仍然是这些最先进的系统的基本要素。离子液体完全由阳离子和阴离子组成,具有多种独特的物理化学和电化学性能,并且具有优异的安全性。本文综述了IL的基本特性、进展和里程碑,以及未来在下一代能源器件中的发展和应用方向。每个部分将全面回顾利用IL电解质的最新进展和技术趋势,重点是Li, Na, k离子电池,金属阳极电池,硫和氧电池,多价金属离子电池和超级电容器,并提到相关的早期研究。与使用传统电解质的系统相比,在每个系统上使用离子液体电解质的好处和相关的性能改进。最后,讨论了离子液体电解质在未来能源器件中的应用前景和挑战。
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引用次数: 16
Interfacial engineering of carbon-based materials for efficient electrocatalysis: Recent advances and future 用于高效电催化的碳基材料界面工程:最新进展与未来
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-05-01 Epub Date: 2022-04-26 DOI: 10.1016/j.enchem.2022.100074
Yu Cheng , Haocong Wang , Tao Qian , Chenglin Yan

Carbon-based materials are widely studied for their unique advantages in electrocatalysis. Despite significant progress, the precise interface construction and mechanism exploration of carbon-based materials in the field of electrocatalysis is still in the early stages. Recently, our group and other peers demonstrated that by introducing heterogeneous components into carbon-based materials, and the forming of specific interfaces will serve as active sites or major reaction sites for electrochemical reactions (OER, HER, ORR, CO2RR, NRR, etc.). Modulating the catalyst interface environment and chemical adsorption behavior through interface engineering is an effective strategy to improve the catalytic activity. This review summarizes the latest progress in the field of carbon-based electrocatalyst in a timely and comprehensive manner, including the classification of carbon-based materials and the interface problems involved, as well as the preparation methods of carbon-based materials in recent years. The interface engineering strategies of carbon-based materials, the structure-activity relationship between interface structure and performance, as well as the potential applications of carbon-based materials in heterogeneous catalytic reactions and energy conversion are discussed in detail. Finally, we outline the current challenges and identify the opportunities facing this emerging sector.

碳基材料因其在电催化方面的独特优势而受到广泛研究。尽管取得了重大进展,但碳基材料在电催化领域的精确界面构建和机理探索仍处于早期阶段。最近,我们课题组和其他同行证明,通过在碳基材料中引入异相组分,并形成特定的界面,将作为电化学反应的活性位点或主要反应位点(OER、HER、ORR、CO2RR、NRR等)。通过界面工程调节催化剂的界面环境和化学吸附行为是提高催化活性的有效策略。本文及时、全面地综述了近年来碳基电催化剂领域的最新进展,包括碳基材料的分类和涉及的界面问题,以及碳基材料的制备方法。详细讨论了碳基材料的界面工程策略、界面结构与性能的构效关系以及碳基材料在非均相催化反应和能量转化中的潜在应用。最后,我们概述了当前的挑战,并确定了这一新兴行业面临的机遇。
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引用次数: 14
Crystalline Porous Materials-based Solid-State Electrolytes for Lithium Metal Batteries 基于晶体多孔材料的锂金属电池固态电解质
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-05-01 Epub Date: 2022-03-23 DOI: 10.1016/j.enchem.2022.100073
Luyi Chen , Kui Ding , Kang Li , Zhongliang Li, Xueliang Zhang, Qifeng Zheng, Yue-Peng Cai, Ya-Qian Lan

The ever-growing market for electric vehicles and grid-scale energy storage is boosting the development of high energy density lithium metal batteries (LMBs). Solid-state electrolytes (SSEs) are not only nonflammable to overcome the intrinsic drawbacks of liquid electrolytes, but also mechanically strong enough to suppress the growth of lithium dendrites, whose development could greatly promote the safety and performance of LMBs. Crystalline porous materials (CPMs) with high surface area, adjustable pores, ordered channels, and versatile functionality have not only provided a promising structural platform for designing fast ionic conducting materials, but also offered great opportunities for manipulating their physicochemical and electrochemical properties, which have shown great potential to fabricate high-performance SSEs and have become an emerging research direction in recent years. In this review, the latest progress of CPMs-based SSEs for LMBs, including pristine CPMs and CPMs-based composites, is systematically summarized. By discussing the pioneer work, both merits and issues arising from CPMs are emphasized as well as an outlook for the development of CPMs-based SSEs with high-performance and reliable safety are presented.

电动汽车和电网规模储能市场的不断增长,推动了高能量密度锂金属电池(lmb)的发展。固态电解质不仅具有不可燃性,克服了液态电解质的固有缺陷,而且具有足够强的机械强度,可以抑制锂枝晶的生长,其发展可以极大地提高lmb的安全性和性能。晶体多孔材料具有高表面积、孔洞可调、通道有序、功能多样等特点,不仅为快速离子导电材料的设计提供了良好的结构平台,而且为控制其物理化学和电化学性能提供了巨大的机会,在制备高性能多孔材料方面显示出巨大的潜力,成为近年来新兴的研究方向。本文系统综述了基于CPMs的lmb复合材料的最新研究进展,包括原始CPMs和复合CPMs。通过对前期工作的讨论,强调了CPMs的优点和存在的问题,并对高性能、安全可靠的基于CPMs的sss的发展进行了展望。
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引用次数: 0
The marriage of two-dimensional materials and phase change materials for energy storage, conversion and applications 二维材料与相变材料的结合用于能量存储、转换和应用
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-03-01 Epub Date: 2022-02-22 DOI: 10.1016/j.enchem.2022.100071
Xiao Chen , Han Yu , Yan Gao , Lei Wang , Ge Wang

Benefiting from high thermal storage density, wide temperature regulation range, operational simplicity, and economic feasibility, latent heat-based thermal energy storage (TES) is comparatively accepted as a cutting-edge TES concept, especially solid-liquid phase change materials (PCMs). However, liquid phase leakage, low thermal/electrical conductivities, weak photoabsorption capacity, and intrinsic rigidity of pristine PCMs are long-standing bottlenecks in both industrial and domestic application scenarios. Towards these goals, emerging two-dimensional (2D) materials containing regions of empty nanospace are ideal alternatives to efficiently encapsulate PCMs molecules and rationalize physical phase transformation, especially graphene, MXene and BN. Herein, we provide a timely and comprehensive review highlighting versatile roles of 2D materials in composite PCMs and relationships between their architectures and thermophysical properties. In addition, we provide an in-depth understanding of the energy conversion mechanisms and rationalize routes to high-efficiency energy conversion PCMs. Finally, we also introduced critical considerations on the challenges and opportunities in the development of advanced high-performance and multifunctional 2D material-based composite PCMs, hoping to provide constructive references and facilitate their significant breakthroughs in both fundamental researches and commercial applications.

基于潜热的热能存储(TES)技术具有储热密度高、温度调节范围宽、操作简单、经济可行等优点,作为一种前沿的热能存储技术,尤其是固液相变材料(PCMs),已被广泛接受。然而,原始PCMs的液相泄漏、低导热/导电性、弱光吸收能力和固有刚性是工业和家庭应用场景中长期存在的瓶颈。为了实现这些目标,新兴的二维(2D)材料包含空纳米空间区域,是有效封装PCMs分子和使物理相变合理化的理想替代品,特别是石墨烯,MXene和BN。在此,我们提供了一个及时和全面的综述,突出了二维材料在复合pcm中的多种作用,以及它们的结构和热物理性质之间的关系。此外,我们还提供了对能量转换机制的深入了解,并合理化了高效能量转换pcm的路线。最后,我们还介绍了先进高性能多功能二维材料基复合PCMs发展面临的挑战和机遇,希望提供建设性的参考,促进其在基础研究和商业应用方面取得重大突破。
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引用次数: 38
Nanostructured Transition Metal Nitrides as Emerging Electrocatalysts for Water Electrolysis: Status and Challenges 纳米结构过渡金属氮化物作为新型水电解电催化剂:现状与挑战
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-03-01 Epub Date: 2022-02-24 DOI: 10.1016/j.enchem.2022.100072
Liwei Lin , Shuqing Piao , Yejung Choi , Lulu Lyu , Hwichan Hong , Dohyeong Kim , Jeongyeon Lee , Wang Zhang , Yuanzhe Piao

Water electrolysis has aroused extensive research efforts due to its potential applications of sewage disposal, microorganism treatment and direct electrolysis for large-scale hydrogen production. At this background, transition metal nitrides (TMNs) have raised lots of attention, because their physical properties are similar to those of metallic elements and TMNs have unique electron orbital structures. The inner nitrogens can increase the electron density of d-bands of transition metals, so that the electronic structures of TMNs are similar with some precious metals, whose density of states can cross the Fermi level. Therefore, TMNs have similar conductivities with metals and possess superior electrocatalytic performance. Nanostructured TMNs tend to have relatively large dispersion and more exposed active sites, which have direct improvement for catalytic activity and stability as electrochemical catalysts. This review summarizes the representative progress of TMNs based catalysts on both synthetic strategies of structural engineering and electronic engineering for improving electrocatalytic performance, especially in hydrogen evolution, oxygen evolution and water splitting. Finally, we further propose the future challenges and research directions of nanostructured TMNs in the electrochemical energy fields of efficient preparations and performance enhancements.

水电解因其在污水处理、微生物处理和直接电解大规模制氢等方面的潜在应用而引起了广泛的研究。在此背景下,过渡金属氮化物(TMNs)因其具有与金属元素相似的物理性质和独特的电子轨道结构而备受关注。内部氮的加入可以增加过渡金属d带的电子密度,使得TMNs的电子结构与某些贵金属相似,其态密度可以跨越费米能级。因此,TMNs具有与金属相似的电导率,具有优越的电催化性能。纳米结构的TMNs往往具有较大的分散性和较多的暴露活性位点,这直接提高了其作为电化学催化剂的催化活性和稳定性。本文从结构工程合成策略和电子工程合成策略两方面综述了具有代表性的TMNs基催化剂在提高电催化性能方面的研究进展,特别是在析氢、析氧和水裂解方面的研究进展。最后,我们进一步提出了纳米结构TMNs在高效制备和性能增强等电化学能量领域面临的挑战和研究方向。
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引用次数: 31
Dealloyed nanoporous materials for electrochemical energy conversion and storage 用于电化学能量转换和存储的合金纳米多孔材料
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2022-01-01 Epub Date: 2022-01-19 DOI: 10.1016/j.enchem.2022.100069
Qinqin Sang , Shuo Hao , Jiuhui Han , Yi Ding

Dealloying, which is traditionally originated in the research of alloy corrosion, has recently been developed as a robust and generic method for fabricating functional 3D nanoporous materials. Endorsed by the unique 3D bicontinuous porous structure, they exhibit remarkable properties such as large surface area, high conductivity, efficient mass transport, and high catalytic activity, which render them as advanced nanomaterials with enormous potential for a variety of applications. In this review, we summarize recent progress in the development of dealloying and dealloyed nanoporous materials for electrochemical energy conversion and storage. Beginning with an overview of the modern understanding of dealloying mechanisms, the unique structural and physical properties of dealloyed nanoporous materials are introduced. Then, we discuss the established dealloying techniques and how they enable the versatile fabrication of a diverse variety of nanoporous materials, ranging from unary metals and alloys to the latest high-entropy alloys and two-dimensional materials. Following that, the electrochemical applications of dealloyed nanoporous materials for fuel cells, supercapacitors, metal-ion batteries, alkali metal batteries, non-aqueous metal-oxygen batteries, electrochemical CO2 reduction, and electrocatalytic N2 reduction are highlighted. Finally, we discuss remaining challenges in this field and offer perspectives on potential directions for future research.

脱合金,传统上起源于合金腐蚀的研究,最近已经发展成为一种强大的和通用的方法来制造功能三维纳米多孔材料。由于具有独特的三维双连续多孔结构,它们具有大表面积、高导电性、高效的传质和高催化活性等显著特性,是一种具有巨大应用潜力的先进纳米材料。本文综述了用于电化学能量转换和存储的脱合金和脱合金纳米多孔材料的研究进展。从对脱合金机制的现代理解的概述开始,介绍了脱合金纳米多孔材料的独特结构和物理性质。然后,我们讨论了已建立的脱合金技术,以及它们如何使各种纳米多孔材料的多用途制造成为可能,从一元金属和合金到最新的高熵合金和二维材料。重点介绍了合金纳米多孔材料在燃料电池、超级电容器、金属离子电池、碱金属电池、非水金属氧电池、电化学CO2还原、电催化N2还原等方面的电化学应用。最后,我们讨论了该领域仍存在的挑战,并对未来的研究方向提出了展望。
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引用次数: 37
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