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Interfacial engineering for high-performance garnet-based lithium metal batteries: A perspective on lithiophilicity and lithiophobicity 高性能石榴石基金属锂电池的界面工程:亲锂性和疏锂性透视
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-01 Epub Date: 2024-03-15 DOI: 10.1016/j.enchem.2024.100122
Pavitra Srivastava , Behrouz Bazri , Dheeraj Kumar Maurya , Wen-Tse Huang , Yu-Kai Liao , Jheng-Yi Huang , Da-Hua Wei , Shu-Fen Hu , Ru-Shi Liu

The research and development of energy storage devices has witnessed a paradigm shift towards the realization of solid-state lithium metal batteries owing to the high theoretical capacity of the lithium metal anode (LMA). Among all types of solid-state electrolytes (SSEs), garnet-based solid electrolytes are one of the most promising candidates which developed due to their relatively high ionic conductivity (10–4 to 10–3 mS cm–1), wide electrochemical stability window (0–6 V vs. Li+/Li), and, most importantly, thermodynamic stability with lithium. Applying suitable interfacial engineering solutions is crucial for solid-state lithium metal batteries, especially for garnet-solid electrolytes due to their brittle nature, which cannot withstand high stack pressure. In this review, we focus on the recent developments in interface engineering solutions and broadly classify them based on the interface modification approach/fabrication routes using various classes of materials. Certain vital electrochemical performance parameters have been compared closely, which gives an appropriate estimation of what types of interlayers will be suitable along with the possible mechanistic route. Moreover, the role of lithium affinity at the interface in terms of lithiophilicity and its importance, along with the presence of lithiophobic phases, is discussed as it amplifies the critical current density of the anode/solid-electrolyte interface and reduces the area-specific resistance. This article comprehensively analyzes the anode-solid-state electrolyte interface in garnet-based lithium metal batteries. It aims to provide a clear perspective on lithiophilicity and lithiophobicity to achieve high-performance batteries.

由于锂金属阳极(LMA)的理论容量较高,储能设备的研究和开发已朝着实现固态锂金属电池的方向发生了范式转变。在所有类型的固态电解质(SSE)中,石榴石基固态电解质因其相对较高的离子电导率(10-4 至 10-3 mS cm-1)、较宽的电化学稳定性窗口(0-6 V 对 Li+/Li)以及最重要的锂热力学稳定性而成为最有前途的候选材料之一。采用合适的界面工程解决方案对于固态锂金属电池来说至关重要,尤其是石榴石固体电解质,因为其性质较脆,无法承受较高的叠加压力。在本综述中,我们将重点介绍界面工程解决方案的最新进展,并根据使用各类材料的界面改性方法/制造路线对其进行大致分类。我们对某些重要的电化学性能参数进行了仔细比较,从而对适合哪种类型的中间膜以及可能的机理路线做出了适当的估计。此外,文章还讨论了亲锂界面上锂亲和性的作用及其重要性,以及疏锂相的存在,因为它能放大阳极/固体-电解质界面的临界电流密度并降低特定区域电阻。本文全面分析了石榴石基锂金属电池中的阳极-固态电解质界面。旨在为实现高性能电池提供一个清晰的亲锂性和疏锂性视角。
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引用次数: 0
Ionic thermoelectric gels and devices: Progress, opportunities, and challenges 离子热电凝胶和器件:进展、机遇与挑战
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-01 Epub Date: 2024-03-19 DOI: 10.1016/j.enchem.2024.100123
Mao Yu , Huan Li , Yuchen Li , Shuaihua Wang , Qikai Li , Yupeng Wang , Benben Li , Kang Zhu , Weishu Liu

Thermoelectric materials are promising in relieving the energy crisis concerning harvesting waste heat and providing a new environment-friendly self-power source for Internet of Things (IoT) sensors. This has attracted significant interest from both the industry and scientific research communities. Fundamentally, general thermoelectric materials are defined as condensed matter that directly converts heat into electricity using electrons or ions as carriers. This review focuses on the emerging ionic thermoelectric (i-TE) gels characterized by distinguished advantages of high voltage output, flexibility, stretchability, and solution processing. Firstly, we systematically review the progress of both p-type and n-type i-TE gels from natural to synthesized gel materials. Secondly, we summarize several strategies for enhancing thermopower, such as entropy engineering, diffusion suppression of counter ions, and several synergistic effects. Thirdly, we briefly review three common modes in which i-TE gels can operate: generator, supercapacitor, and cycle mode. Fourthly, we discussed the effect of electrode structure and gel structure on the energy output. We also highlight the opportunity for i-TE gels to explore new applications based on their unique advantages. Finally, the challenges and perspectives are presented, suggesting a challenging technique road and a bright future in this emerging field.

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引用次数: 0
Tuning the local coordination environment of single-atom catalysts for enhanced electrocatalytic activity 调节单原子催化剂的局部配位环境以提高电催化活性
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-03-01 Epub Date: 2024-02-17 DOI: 10.1016/j.enchem.2024.100119
Wenhao Feng , Chunli Liu , Guangxun Zhang , Hui Yang , Yichun Su , Yangyang Sun , Huan Pang

The local coordination environment (LCE) plays a pivotal role in determining catalyst performance. By controlling the LCE of catalysts, the catalytic activity, selectivity, and stability of catalysts can be effectively increased. This influence is particularly pronounced in the realm of electrocatalysis, especially for single-atom catalysts (SACs). However, it is still a challenge to properly regulate the LCE and improve the activity and stability of SACs during catalysis. According to the differences in electron distribution and interaction between atoms in different types of chemical bonds, the LCE can be adjusted by experimental and simulated design. In this review, we discuss the characterization of LCE in SACs, explore the impact of adjusting LCE in high-performance electrocatalysts and summarize the challenges and opportunities of SACs in the future. We aim for this review to provide new insights into further research on SACs.

局部配位环境(LCE)在决定催化剂性能方面起着举足轻重的作用。通过控制催化剂的 LCE,可以有效提高催化剂的催化活性、选择性和稳定性。这种影响在电催化领域尤为明显,尤其是单原子催化剂(SAC)。然而,如何在催化过程中适当调节 LCE 并提高 SAC 的活性和稳定性仍是一项挑战。根据不同类型化学键中电子分布和原子间相互作用的差异,可以通过实验和模拟设计来调节 LCE。在这篇综述中,我们讨论了 SACs 中 LCE 的表征,探讨了调整 LCE 对高性能电催化剂的影响,并总结了 SACs 未来面临的挑战和机遇。我们希望本综述能为 SAC 的进一步研究提供新的见解。
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引用次数: 0
Design strategies of iridium(III) complexes for highly efficient saturated blue phosphorescent OLEDs with improved lifetime 铱(III)配合物的设计策略,用于提高寿命的高效饱和蓝色磷光 OLED
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-03-01 Epub Date: 2024-02-27 DOI: 10.1016/j.enchem.2024.100120
Chengcheng Wu , Kefei Shi , Siqi Li , Jie Yan , Zi-Qi Feng , Kai-Ning Tong , Si-Wei Zhang , Yuewei Zhang , Dongdong Zhang , Liang-Sheng Liao , Yun Chi , Guodan Wei , Feiyu Kang

This review explores the latest advancements of iridium(III) phosphorescent blue emitters by focusing on the design strategies employed for saturated blue phosphorescent OLEDs with enhanced operational lifetime. Saturated blue emission remains a challenging aspect of OLED technology, and iridium(III) complexes have emerged as promising materials to address this issue. The molecular design principles, ligand engineering and host materials that facilitate the achievement of highly efficient blue phosphorescent emission are explored. Additionally, various host-guest systems and device architectures that have been employed to prolong the operational lifetime of these OLEDs are systematically examined. The review highlights recent breakthroughs and prospects, including the synthesis of novel iridium(III) complexes, advanced device engineering strategies, and potential application in next-generation displays and lighting technologies. Therefore, this comprehensive analysis serves as a valuable resource for researchers and industry professionals engaged in the development of advanced OLEDs with improved efficiency and longevity.

这篇综述探讨了铱(III)磷光蓝光发射器的最新进展,重点介绍了具有更长工作寿命的饱和蓝光有机发光二极管所采用的设计策略。饱和蓝色发射仍然是有机发光二极管技术的一个挑战,而铱(III)配合物已成为解决这一问题的有前途的材料。本文探讨了有助于实现高效蓝色磷光发射的分子设计原理、配体工程和宿主材料。此外,还系统研究了用于延长这些有机发光二极管工作寿命的各种主-客体系统和器件架构。综述重点介绍了最近的突破和前景,包括新型铱(III)配合物的合成、先进的器件工程策略以及在下一代显示和照明技术中的潜在应用。因此,这篇全面的分析报告对于从事先进有机发光二极管开发的研究人员和行业专业人士来说,是一份宝贵的资源,可提高发光二极管的效率和寿命。
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引用次数: 0
Covalent organic frameworks for efficient hydrogen peroxide production 用于高效生产过氧化氢的共价有机框架
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-03-01 DOI: 10.1016/j.enchem.2024.100121
Ting He, Yanli Zhao

The field of hydrogen peroxide (H2O2) has attracted enormous interests because H2O2 is a sort of environmental-friendly oxidant to be widely used in sanitation, chemical industry and environmental field. The high energy consumption and production of harmful by-product waste of conventional anthraquinone oxidation technology calls for the development of green and sustainable technologies for H2O2 production. The photocatalytic and electrocatalytic H2O2 production based on the covalent organic framework (COF) catalysts has been developed rapidly during the past few years due to the advantages of COFs including structural designability, high crystallinity, good porosity and stability. In this review, the basic principles, recent achievements and strategies for the design of COF photocatalysts and electrocatalysts to improve the performance of H2O2 production are summarized and highlighted. The challenges and perspective for the future directions are discussed in detail. This review is expected to pave the way for the rational design of advanced COF catalysts for the sustainable H2O2 production.

过氧化氢(H2O2)是一种环境友好型氧化剂,可广泛应用于卫生、化工和环境领域,因此该领域备受关注。传统的蒽醌氧化技术能耗高且会产生有害的副产品废物,因此需要开发绿色和可持续的 H2O2 生产技术。基于共价有机框架(COF)催化剂的光催化和电催化 H2O2 生产技术,由于 COF 具有结构可设计、结晶度高、孔隙率和稳定性好等优点,在过去几年得到了快速发展。本综述总结并重点介绍了 COF 光催化剂和电催化剂设计的基本原理、最新成果和策略,以提高 H2O2 的生产性能。此外,还详细讨论了未来发展方向所面临的挑战和前景。本综述有望为合理设计可持续生产 H2O2 的先进 COF 催化剂铺平道路。
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引用次数: 0
Crystal nano-engineering: A new era for perovskite photovoltaics 晶体纳米工程:包晶光伏的新时代
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-03-01 Epub Date: 2024-02-03 DOI: 10.1016/j.enchem.2024.100118
Francesco Lamberti , Teresa Gatti
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引用次数: 0
Recent advances in the surface modification strategies towards 3D carbon-based hosts for dendrite-free Li/Na/Zn metal anodes 无树枝状锂/镍/锌金属阳极的三维碳基宿主表面改性策略的最新进展
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-03-01 Epub Date: 2024-01-30 DOI: 10.1016/j.enchem.2024.100117
Chen Chen, Nian Wu Li, Le Yu

Rechargeable Li/Na/Zn metal batteries are promising next-generation energy-storage systems owing to their high energy density. However, the inhomogeneous deposition behavior, severe dendrite growth and drastic volume variation hinder the practical applications of Li/Na/Zn metal anodes. Three-dimensional (3D) carbon-based substrates have received extensive attention in view of their low cost, high electronic conductivity, and adjustable physicochemical characteristic. Moreover, their interconnected network architecture can accommodate the enormous internal stress fluctuation, homogenize electric field distribution, and mitigate Li/Na/Zn dendrite growth. Herein, we review the recent advances in 3D carbon-based hosts employing surface modification strategies to accomplish spatially confined deposition behavior of metallic Li/Na/Zn. Firstly, self-templated synthesis and hard-templating synthesis for manufacturing the 3D carbon-based scaffolds are briefly presented. Subsequently, we investigate several typical surface modification strategies, including heteroatom doping, surface functionalization, decoration of nucleation sites, and skeleton gradient design of metallophilicity and electronic conductivity. Finally, the future perspectives on several research orientations for the commercial application of 3D carbon-based hosts as metal anodes are emphasized.

可充电锂/钽/锌金属电池因其高能量密度而成为前景广阔的下一代储能系统。然而,不均匀沉积行为、严重的枝晶生长和剧烈的体积变化阻碍了锂/镍/锌金属阳极的实际应用。三维碳基衬底因其低成本、高电子传导性和可调节的物理化学特性而受到广泛关注。此外,它们相互连接的网络结构可以适应巨大的内部应力波动、均匀电场分布并减缓锂/镍/锌枝晶的生长。在此,我们回顾了利用表面改性策略实现金属锂/钽/锌空间约束沉积行为的三维碳基宿主的最新进展。首先,我们简要介绍了用于制造三维碳基支架的自模板合成和硬模板合成。随后,我们研究了几种典型的表面改性策略,包括杂原子掺杂、表面功能化、成核点装饰以及亲金属性和电子导电性的骨架梯度设计。最后,我们强调了三维碳基宿主作为金属阳极的商业应用的几个研究方向的未来前景。
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引用次数: 0
Metal-organic framework composites for photocatalysis 光催化用金属-有机框架复合材料
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-01-01 Epub Date: 2023-11-22 DOI: 10.1016/j.enchem.2023.100115
Di Chen , Yu-Tao Zheng , Ning-Yu Huang , Qiang Xu

In the past decades, metal-organic frameworks (MOFs) have gained great attention as a promising candidate in photocatalytic applications, leveraging their tunable pores, well-defined structures, ease of functionalization and inherent semiconductor properties. Nevertheless, owing to their poor light-harvesting capability and suboptimal electron-hole separation efficiency, their catalytic performances have yet to meet the prerequisites for industrial deployment. To address this issue, researchers started to incorporate guest substances into MOFs, thereby integrating multiple functions or advantages to form MOF composites. Through the construction of active interfaces and the introduction of functional units, the light absorption capacity, charge separation and the reaction activity are pointedly optimized, thus enhancing the overall photocatalytic performances. Moreover, the composites exhibit various active sites with well-defined coordination configuration, facilitating the study of the photocatalytic mechanism. Herein, this review provides an overview of commonly used MOF composites in photocatalysis, including metal nanoparticles/MOFs, semiconductors/MOFs, carbon materials/MOFs, aerogels/MOFs, polymers/MOFs, reticular frameworks/MOFs, and MOF composites with others, summarizes their synthesis strategies, and presents their latest applications in photocatalytic water splitting, CO2 reduction, N2 reduction and organic reactions. We hope that this review will highlight the advantages and challenges of MOF composites in photocatalysis and inspire the development of more efficient and widely applicable novel MOF composite photocatalysts.

在过去的几十年里,金属有机框架(mof)由于其可调节的孔、明确的结构、易于官能化和固有的半导体特性,在光催化应用中获得了广泛的关注。然而,由于其较差的光收集能力和次优的电子-空穴分离效率,其催化性能尚未满足工业部署的先决条件。为了解决这一问题,研究人员开始将客体物质加入到MOF中,从而集成多种功能或优点,形成MOF复合材料。通过活性界面的构建和功能单元的引入,有针对性地优化了光吸收能力、电荷分离和反应活性,从而提高了整体的光催化性能。此外,复合材料具有多种活性位点和明确的配位构型,有利于光催化机理的研究。本文综述了光催化中常用的MOF复合材料,包括金属纳米颗粒/MOF、半导体/MOF、碳材料/MOF、气凝胶/MOF、聚合物/MOF、网状框架/MOF以及MOF复合材料等,综述了它们的合成策略,并介绍了它们在光催化水裂解、CO2还原、N2还原和有机反应中的最新应用。希望本文综述能够突出MOF复合材料在光催化方面的优势和挑战,为开发出更高效、更广泛应用的新型MOF复合光催化剂提供参考。
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引用次数: 0
Donor-acceptor-based conjugated polymers for photocatalytic energy conversion 用于光催化能量转换的给体-受体共轭聚合物
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-01-01 Epub Date: 2023-11-29 DOI: 10.1016/j.enchem.2023.100116
Chao Yang , Bei Cheng , Jingsan Xu , Jiaguo Yu , Shaowen Cao

Photocatalytic solar-to-chemical energy conversion is deemed to be a promising, eco-friendly, and low-energy input strategy for addressing the energy crisis. Donor−acceptor (D−A) conjugated polymers (CPs) have recently emerged as the hub in photocatalysis due to their charming properties, such as variable molecular structure, accessible functionalization, tunable electronic band structure, and versatile synthetic approaches. These features enable D−A-based CPs to be a potential alternative for conventional inorganic photocatalysts. Currently, researchers are making great efforts to design highly-efficient D−A-based CPs for adaptable photocatalytic reactions. In this review, the development, classification, and common synthetic strategies of D−A-based CPs are introduced. The recent progress of D−A-based CPs in photocatalytic energy conversion is systematically summarized, including photocatalytic H2 evolution, O2 evolution, overall water splitting, CO2 reduction, H2O2 production, and organic transformation. Meanwhile, the impacts of molecular/electronic structure and morphology of D−A-based CPs on light-harvesting capacity, exciton dissociation, and interfacial reaction during the photo-redox reactions are clarified. Finally, the conclusions and future challenges for photocatalytic energy conversion over D−A-based CPs are provided. This review is expected to offer an in-depth and comprehensive understanding of photocatalytic energy conversion in the aspect of mechanism, as well as to stimulate inspiration for designing D−A-based CP photocatalysts with surpassing efficiency.

光催化太阳能-化学能源转换被认为是解决能源危机的一种有前途的、环保的、低能源投入的战略。供体-受体(D - A)共轭聚合物(CPs)由于其独特的特性,如可变的分子结构、可获得的功能化、可调谐的电子带结构和通用的合成方法,近年来成为光催化领域的中心。这些特点使D -基CPs成为传统无机光催化剂的潜在替代品。目前,研究人员正在努力设计用于适应性光催化反应的高效D -基CPs。本文综述了D -基CPs的发展、分类和常用的合成策略。系统综述了D -基CPs在光催化能量转化方面的最新进展,包括光催化析H2、析O2、整体水分解、CO2还原、H2O2生成和有机转化。同时,阐明了D -基CPs的分子/电子结构和形态对光氧化还原反应中光捕获能力、激子解离和界面反应的影响。最后,提出了D -基CPs光催化能量转换的结论和未来的挑战。本文的综述将为深入、全面地了解光催化能量转换的机理提供参考,并为设计具有卓越效率的D−基CP光催化剂提供启示。
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引用次数: 0
Elevated temperature adsorbents for separation applications 用于分离应用的高温吸附剂
IF 25.1 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-11-01 Epub Date: 2023-11-20 DOI: 10.1016/j.enchem.2023.100113
Shuang Li , Xuancan Zhu , Dongdong Wang , Peixuan Hao , Fangzhe Zhou , Yixiang Shi , Ruzhu Wang , Ningsheng Cai

Elevated-temperature adsorptive separation involves the selective and rapid adsorption of gas molecules on weakly bonding chemical sites of an adsorbent at elevated temperatures (80–500 °C) and the reversible desorption of the gas molecules at a low cost. It is a significant step in several reactions, such as pre-combustion carbon capture, indirect/direct hydrogen production, ammonia separation, oxygen production from air, and carbon monoxide enrichment. This purification strategy avoids sensible heat loss of the feed gas, heat regeneration, accelerates adsorption kinetics, and can sometimes couple catalysts to achieve sorption-enhanced reactions. Before commercializing elevated-temperature adsorptive separation technologies, highly efficient syntheses for obtaining elevated-temperature-responsive adsorbents are required; competitive adsorption, interactions with gas impurities, and poisoning mechanisms need to be well understood; specific adsorption reactors and processes should also be designed. Therefore, this review covers the key progress made in terms of material design and synthesis, adsorption kinetic models and mechanisms, process design and optimization, as well as system integration for elevated-temperature adsorptive separation. This review will be valuable for the clean fossil-fuel utilization community, as well as energy and chemical industries.

高温吸附分离涉及在高温(80-500℃)下,气体分子在吸附剂的弱键化学位点上的选择性和快速吸附,以及气体分子的低成本可逆解吸。它是几个反应的重要步骤,如燃烧前碳捕获、间接/直接制氢、氨分离、空气制氧和一氧化碳富集。这种净化策略避免了原料气的显热损失,热再生,加速吸附动力学,有时可以耦合催化剂来实现吸附增强反应。在高温吸附分离技术商业化之前,需要高效合成高温响应吸附剂;竞争性吸附、与气体杂质的相互作用和中毒机制需要充分了解;还应设计特定的吸附反应器和工艺。本文综述了高温吸附分离在材料设计与合成、吸附动力学模型与机理、工艺设计与优化、系统集成等方面的研究进展。该综述对清洁化石燃料利用界以及能源和化学工业具有一定的参考价值。
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引用次数: 0
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