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Progress in metal oxide-based electrocatalysts for sustainable water splitting 基于金属氧化物的可持续水分离电催化剂研究进展
Pub Date : 2024-08-01 DOI: 10.1016/j.matre.2024.100283
Aasiya S. Jamadar, Rohit Sutar, Susmita Patil, Reshma Khandekar, Jyotiprakash B. Yadav

Metal oxide-based electrocatalysts are promising alternatives to platinum group metals for water splitting due to their low cost, abundant raw materials, and impressive stability. This review covers recent progress in various metal oxides tailored for hydrogen and oxygen evolution reactions, discussing their crystal structure, composition, and surface modification influence on performance. Strategies like surface engineering, doping, and nanostructuring are evaluated for enhancing catalytic activity and stability. The key considerations for commercialization are highlighted, emphasizing ongoing research, innovation, and future scope to drive widespread adoption of water-splitting technology for a cleaner and sustainable future.

基于金属氧化物的电催化剂因其成本低廉、原材料丰富和令人印象深刻的稳定性,有望成为铂族金属的水分离替代品。这篇综述涵盖了为氢和氧进化反应量身定制的各种金属氧化物的最新进展,讨论了它们的晶体结构、组成和表面改性对性能的影响。对表面工程、掺杂和纳米结构等策略进行了评估,以提高催化活性和稳定性。重点介绍了商业化的主要考虑因素,强调了正在进行的研究、创新和未来的发展空间,以推动水分离技术的广泛应用,实现更清洁和可持续发展的未来。
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引用次数: 0
Outside Back Cover 封底外侧
Pub Date : 2024-08-01 DOI: 10.1016/S2666-9358(24)00061-2
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引用次数: 0
An organic visible-photocatalytic-adsorbence mechanism to high-efficient removal of heavy metal antimony ions 高效去除重金属锑离子的有机可见光催化吸附机制
Pub Date : 2024-08-01 DOI: 10.1016/j.matre.2024.100284
Linji Yang , Ke Sun , Tao Liu , Ciyuan Huang , Libin Zhang , Yang Zhou , Kai Chen , Shangfei Yao , Ziyang Zhang , Chenfu Zhao , Hongxiang Zhu , Bingsuo Zou , Shuangfei Wang , Dongfeng Xue

Purification of emerging heavy metal antimony contaminated water based on advanced ingenious strategies. An activated modified coconut shell charcoal (CSC) was synthesized and evaluated as a substrate-supported loaded organic photovoltaic material, PM6:PYIT:PM6-b-PYIT, to prepare a surprisingly highly efficient, stable, environmentally friendly, and recyclable organic photocatalyst (CSC–N–P.P.P), which showed excellent effects on the simultaneous removal of Sb(III) and Sb(V). The removal efficiency of CSC-N-P.P.P on Sb(Ⅲ) and Sb(V) reached an amazing 99.9% in quite a short duration of 15 min. At the same time, under ppb level and indoor visible light (∼1 W m−2), it can be treated to meet the drinking water standards set by the European Union and the U.S. National Environmental Protection Agency in 5 min, and even after 25 cycles of recycling, the efficiency is still maintained at about 80%, in addition to the removal of As (III), Cd (II), Cr (VI), and Pb (II) can also be realized. The catalyst not only solves the problems of low reuse rate, difficult structure adjustment and high energy consumption of traditional photocatalysts but also has strong applicability and practical significance. The pioneering approach provides a much-needed solution strategy for removing highly toxic heavy metal antimony pollution from the environment.

利用先进的巧妙策略净化新出现的重金属锑污染水。合成并评估了一种活性改性椰壳炭(CSC)作为基底支撑的负载有机光电材料--PM6:PYIT:PM6-b-PYIT,制备出一种高效、稳定、环保、可回收的有机光催化剂(CSC-N-P.P.P),该催化剂在同时去除Sb(Ⅲ)和Sb(V)方面表现出卓越的效果。在很短的 15 分钟内,CSC-N-P.P.P 对 Sb(Ⅲ)和 Sb(V)的去除率达到了惊人的 99.9%。同时,在ppb级和室内可见光(∼1 W m-2)条件下,5分钟内即可处理达到欧盟和美国国家环境保护局规定的饮用水标准,即使经过25次循环处理,效率仍能保持在80%左右,此外还能实现对As (III)、Cd (II)、Cr (VI)和Pb (II)的去除。该催化剂不仅解决了传统光催化剂重复利用率低、结构调整难、能耗高等问题,而且具有很强的应用性和现实意义。这一开创性的方法为清除环境中剧毒重金属锑污染提供了亟需的解决策略。
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引用次数: 0
A triboelectric nanogenerator based on a spiral rotating shaft for efficient marine energy harvesting of the hydrostatic pressure differential 一种基于螺旋旋转轴的三电纳米发电机,可高效采集海洋静水压差能量
Pub Date : 2024-08-01 DOI: 10.1016/j.matre.2024.100280

Equipment used in underwater sensing and exploration typically relies on cables or batteries for energy supply, resulting in a limited and inconvenient energy supply and marine environmental pollution that hinder the sustainable development of distributed ocean sensing networks. Here, we design a deep-sea differential-pressure triboelectric nanogenerator (DP-TENG) based on a spiral shaft drive using modified polymer materials to harness the hydrostatic pressure gradient energy at varying ocean depths to power underwater equipment. The spiral shaft structure converts a single compression into multiple rotations of the TENG rotor, achieving efficient conversion of differential pressure energy. The multi-pair electrode design enables the DP-TENG to generate a peak current of 61.7 μA, the instantaneous current density can reach 0.69 μA cm−2, and the output performance can be improved by optimizing the spiral angle of the shaft. The DP-TENG can charge a 33 μF capacitor to 17.5 V within five working cycles. It can also power a digital calculator and light up 116 commercial power light-emitting diodes, demonstrating excellent output capability. With its simple structure, low production cost, and small form factor, the DP-TENG can be seamlessly integrated with underwater vehicles. The results hold broad prospects for underwater blue energy harvesting and are expected to contribute to the development of self-powered equipment toward emerging “smart ocean” and blue economy applications.

用于水下传感和勘探的设备通常依靠电缆或电池提供能源,导致能源供应有限且不方便,并造成海洋环境污染,阻碍了分布式海洋传感网络的可持续发展。在此,我们设计了一种基于螺旋轴驱动的深海压差三电纳米发电机(DP-TENG),使用改性聚合物材料,利用不同海洋深度的静水压力梯度能量为水下设备供电。螺旋轴结构将一次压缩转换为 TENG 转子的多次旋转,实现了压差能的高效转换。多对电极设计使 DP-TENG 能够产生 61.7 μA 的峰值电流,瞬时电流密度可达 0.69 μA cm-2,并可通过优化轴的螺旋角度提高输出性能。DP-TENG 可在五个工作周期内将一个 33 μF 的电容器充电至 17.5 V。它还能为数字计算器供电,并点亮 116 个商用功率发光二极管,显示出卓越的输出能力。DP-TENG 结构简单、生产成本低、外形小巧,可与水下航行器无缝集成。该成果为水下蓝色能量采集带来了广阔的前景,有望推动自供电设备的发展,实现新兴的 "智慧海洋 "和蓝色经济应用。
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引用次数: 0
S-doped mesoporous graphene modified separator for high performance lithium-sulfur batteries 用于高性能锂硫电池的 S 掺杂介孔石墨烯改性隔膜
Pub Date : 2024-08-01 DOI: 10.1016/j.matre.2024.100279
Xinlong Ma , Chenggen Xu , Yin Yang , Dong Sun , Kai Zhao , Changbo Lu , Peng Jin , Yiting Chong , Sirawit Pruksawan , Zhihua Xiao , Fuke Wang

Due to their low cost, environmental friendliness and high energy density, the lithium-sulfur batteries (LSB) have been regarded as a promising alternative for the next generation of rechargeable battery systems. However, the practical application of LSB is seriously hampered by its short cycle life and high self-charge owing to the apparent shuttle effect of soluble lithium polysulfides. Using MgSO4@MgO composite as both template and dopant, template-guided S-doped mesoporous graphene (SMG) is prepared via the fluidized-bed chemical vapor deposition method. As the polypropylene (PP) modifier, SMG with high specific surface area, abundant mesoporous structures and moderate S doping content offers a wealth of physical and chemical adsorptive sites and reduced interfacial contact resistance, thereby restraining the serious shuttle effects of lithium polysulfides. Consequently, the LSB configured with mesoporous graphene (MG) as S host material and SMG as a separator modifier exhibits an enhanced electrochemical performance with a high average capacity of 955.64 mA h g−1 at 1C and a small capacity decay rate of 0.109% per cycle. Additionally, the density functional theory (DFT) calculation models have been rationally constructed and demonstrated that the doped S atoms in SMG possess higher binding energy to lithium polysulfides than that in MG, indicating that the SMG/PP separator can effectively capture soluble lithium polysulfides via chemical binding forces. This work would provide valuable insight into developing a versatile carbon-based separator modifier for LSB.

锂硫电池(LSB)具有成本低、环保和能量密度高等优点,被视为下一代充电电池系统的理想替代品。然而,由于可溶性锂多硫化物的明显穿梭效应,锂硫电池的循环寿命短和高自充电率严重阻碍了其实际应用。利用 MgSO4@MgO 复合材料作为模板和掺杂剂,通过流化床化学气相沉积法制备了模板引导的 S 掺杂介孔石墨烯(SMG)。作为聚丙烯(PP)的改性剂,SMG 具有高比表面积、丰富的介孔结构和适度的 S 掺杂含量,可提供丰富的物理和化学吸附位点并降低界面接触电阻,从而抑制多硫化锂的严重穿梭效应。因此,以介孔石墨烯(MG)为 S 主材料、SMG 为分离改性剂的 LSB 具有更高的电化学性能,在 1C 时的平均容量高达 955.64 mA h g-1,且每周期的容量衰减率仅为 0.109%。此外,合理构建的密度泛函理论(DFT)计算模型表明,SMG 中掺杂的 S 原子与多硫化锂的结合能高于 MG,表明 SMG/PP 分离剂可通过化学结合力有效捕获可溶性多硫化锂。这项工作将为开发用于 LSB 的多功能碳基分离改性剂提供宝贵的见解。
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引用次数: 0
Recent advances in single-atom catalysts (SACs) for photocatalytic applications 用于光催化应用的单原子催化剂 (SAC) 的最新进展
Pub Date : 2024-08-01 DOI: 10.1016/j.matre.2024.100285
Tingcha Wei , Jing Zhou , Xiaoqiang An

Artificial photocatalysis represents a hopeful avenue for tackling the global crisis of environmental and energy sustainability. The crux of industrial application in photocatalysis lies in efficient photocatalysts that can inhibit the recombination of photogenerated charge carriers, thereby boost the efficiency of chemical reactions. In the past decade, single-atom catalysts (SACs) have been growing extremely rapidly and have become the forefront of photocatalysis owing to their superior utilization of metal atoms and outstanding catalytic activity. In this work, we provide an overview of the latest advancements and challenges in SACs for photocatalysis, focusing on the photocatalytic mechanisms, encompassing the generation, separation, migration, and surface extraction of photogenerated carriers. We also explore the design, synthesis, and characterization of SACs and introduce the progress of SACs for photocatalytic applications, such as water splitting and CO2 reduction. Lastly, we offer our personal perspectives on the opportunities and challenges of SACs in photocatalysis, aiming to provide insights into the future studies of SACs for photocatalytic applications.

人工光催化是解决全球环境和能源可持续发展危机的一条充满希望的途径。光催化工业应用的关键在于高效的光催化剂,它可以抑制光生电荷载流子的重组,从而提高化学反应的效率。近十年来,单原子催化剂(SAC)发展极为迅速,由于其金属原子利用率高、催化活性突出,已成为光催化领域的前沿技术。在这项工作中,我们概述了用于光催化的单原子催化剂的最新进展和挑战,重点是光催化机理,包括光生载体的生成、分离、迁移和表面萃取。我们还探讨了 SAC 的设计、合成和表征,并介绍了 SAC 在光催化应用(如水分离和二氧化碳还原)方面的进展。最后,我们就 SACs 在光催化领域的机遇和挑战提出了个人观点,旨在为今后研究 SACs 在光催化领域的应用提供启示。
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引用次数: 0
Advancements in biomass gasification research utilizing iron-based oxygen carriers in chemical looping: A review 在化学循环中利用铁基氧载体的生物质气化研究进展:综述
Pub Date : 2024-08-01 DOI: 10.1016/j.matre.2024.100282
Yonghong Niu , Zhengyang Chi , Ming Li

Biomass, recognized as renewable green coal, is pivotal for energy conservation, emission reduction, and dual-carbon objectives. Chemical looping gasification, an innovative technology, aims to enhance biomass utilization efficiency. Using metal oxides as oxygen carriers regulates the oxygen-to-fuel ratio to optimize synthesis product yields. This review examines various oxygen carriers and their roles in chemical looping biomass gasification, including natural iron ore types, industrial by-products, cerium oxide-based carriers, and core-shell structures. The catalytic, kinetic, and phase transfer properties of iron-based oxygen carriers are analyzed, and their catalytic cracking capabilities are explored. Molecular interactions are elucidated and system performance is optimized by providing insights into chemical looping reaction mechanisms and strategies to improve carrier efficiency, along with discussing advanced techniques such as density functional theory (DFT) and reactive force field (ReaxFF) molecular dynamics (MD). This paper serves as a roadmap for advancing chemical looping gasification towards sustainable energy goals.

生物质是公认的可再生绿色煤炭,在实现节能减排和双碳目标方面具有举足轻重的作用。化学循环气化是一项创新技术,旨在提高生物质的利用效率。使用金属氧化物作为氧载体可以调节氧与燃料的比例,从而优化合成产品的产量。本综述探讨了各种氧载体及其在化学循环生物质气化中的作用,包括天然铁矿石类型、工业副产品、基于氧化铈的载体以及核壳结构。分析了铁基氧载体的催化、动力学和相转移特性,并探讨了它们的催化裂解能力。通过深入探讨化学循环反应机制和提高载体效率的策略,以及讨论密度泛函理论 (DFT) 和反应力场 (ReaxFF) 分子动力学 (MD) 等先进技术,阐明了分子间的相互作用,并优化了系统性能。本文是推动化学循环气化技术实现可持续能源目标的路线图。
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引用次数: 0
Synthesis of nanostructured zinc oxide and its composite with carbon dots for DSSCs applications using flexible electrode 利用柔性电极合成用于 DSSC 应用的纳米结构氧化锌及其与碳点的复合材料
Pub Date : 2024-08-01 DOI: 10.1016/j.matre.2024.100281

ZnO nanowires (ZnO NWs), ZnO nanoparticles (ZnO NPs) and carbon dots (C-dots) were synthesized by hydrothermal, sol-gel and hydrothermal methods respectively. They were also characterized and applied for dye sensitized solar cells (DSSCs). The effects of C-dots on ZnO NWs and ZnO NPs have been evaluated. The C-dots were used at a mole ratio of citric acid (CA) to ethylene diamine (EDA) of 1 : 1.5. These C-dots were found to enhance the performance of the flexible electrode DSSCs. After the addition of C-dots, the power conversion efficiency (PCE) of ZnO NPs was boosted to be two times higher than that of ZnO NPs DSSCs without C-dots. Similarly, the ultraviolet (UV)-band revealed a blue shift, resulting in a lower band gap and a reduced charge transfer resistance, which can enhance the PCE of DSSCs. The loaded quantity on the flexible electrode substrate made of polyethylene terephthalate (PET) was optimized (50 mg). For DSSCs, the PET flexible electrode conductive polymer has produced positive outcomes. For ZnO NWs and ZnO NWs@C-dots, the PCE values were 1.45% and 4.25%; while for ZnO NPs and ZnO NPs@C-dots, they were 2.34% and 5.81%, respectively. This work achieved remarkable and competitive performance when compared to solid (indium tin oxides/glass)-based substrate.

采用水热法、溶胶-凝胶法和水热法分别合成了氧化锌纳米线(ZnO NWs)、氧化锌纳米颗粒(ZnO NPs)和碳点(C-dots)。研究还对它们进行了表征,并将其应用于染料敏化太阳能电池(DSSC)。评估了 C 点对 ZnO NWs 和 ZnO NPs 的影响。柠檬酸(CA)与乙二胺(EDA)的摩尔比为 1:1.5。研究发现,这些 C 点可提高柔性电极 DSSC 的性能。添加 C 点后,氧化锌氮氧化物的功率转换效率(PCE)比不添加 C 点的氧化锌氮氧化物 DSSC 高出两倍。同样,紫外(UV)带出现蓝移,导致带隙降低,电荷转移电阻减小,从而提高了 DSSC 的 PCE。聚对苯二甲酸乙二醇酯(PET)制成的柔性电极基底上的负载量进行了优化(50 毫克)。对于 DSSC 而言,PET 柔性电极导电聚合物产生了积极的效果。ZnO NWs 和 ZnO NWs@C-dots 的 PCE 值分别为 1.45% 和 4.25%;而 ZnO NPs 和 ZnO NPs@C-dots 的 PCE 值分别为 2.34% 和 5.81%。与基于固体(铟锡氧化物/玻璃)的基底相比,这项工作取得了卓越的性能和竞争力。
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引用次数: 0
Unraveling the coordination behavior and transformation mechanism of Cr3+ in Fe–Cr redox flow battery electrolytes 揭示铁-铬氧化还原液流电池电解质中 Cr3+ 的配位行为和转化机制
Pub Date : 2024-05-01 DOI: 10.1016/j.matre.2024.100271
Xiaojun Zhao , Xinwei Niu , Xinyuan Liu , Chongchong Wu , Xinyu Duan , Zhiqi Ma , Yan Xu , Hao Li , Weijie Yang

Currently, the iron chromium redox flow battery (ICRFB) has become a research hotspot in the energy storage field owing to its low cost and easily-scaled-up. However, the activity of electrolyte is still ambiguous due to its complicated solution environment. Herein, we performed a pioneering investigation on the coordination behavior and transformation mechanism of Cr3+ in electrolyte and prediction of impurity ions impact through quantum chemistry computations. Based on the structure and symmetry of electrostatic potential distribution, the activity of different Cr3+ complex ions is confirmed as [Cr(H2O)5Cl]2+ > [Cr(H2O)4Cl2]+ > [Cr(H2O)6]3+. The transformation mechanism between [Cr(H2O)6]3+ and [Cr(H2O)5Cl]2+ is revealed. We find the metal impurity ions (especially Mg2+) can exacerbate the electrolyte deactivation by reducing the transformation energy barrier from [Cr(H2O)5Cl]2+ (24.38 kcal mol−1) to [Cr(H2O)6]3+ (16.23 kcal mol−1). The solvent radial distribution and mean square displacement in different solvent environments are discussed and we conclude that the coordination configuration limits the diffusivity of Cr3+. This work provides new insights into the activity of electrolyte, laying a fundamental sense for the electrolyte in ICRFB.

目前,铁铬氧化还原液流电池(ICRFB)因其成本低、易于规模化生产而成为储能领域的研究热点。然而,由于其复杂的溶液环境,电解质的活性仍不明确。在此,我们开创性地研究了 Cr3+ 在电解质中的配位行为和转化机制,并通过量子化学计算预测了杂质离子的影响。根据静电位分布的结构和对称性,确定了[Cr(H2O)5Cl]2+ >;[Cr(H2O)4Cl2]+ >;[Cr(H2O)6]3+等不同Cr3+配合离子的活性。揭示了 [Cr(H2O)6]3+ 和 [Cr(H2O)5Cl]2+ 之间的转化机制。我们发现金属杂质离子(尤其是 Mg2+)会降低从 [Cr(H2O)5Cl]2+ (24.38 kcal mol-1)到 [Cr(H2O)6]3+ (16.23 kcal mol-1)的转化能垒,从而加剧电解质失活。我们讨论了不同溶剂环境中的溶剂径向分布和均方位移,并得出结论:配位限制了 Cr3+ 的扩散性。这项研究为了解电解质的活性提供了新的视角,为 ICRFB 中的电解质奠定了基础。
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引用次数: 0
Carboxylic bacterial cellulose fiber-based hydrogel electrolyte with imidazole-type ionic liquid for dendrite-free zinc metal batteries 基于羧基细菌纤维素纤维的水凝胶电解质与咪唑类离子液体,用于无枝晶型锌金属电池
Pub Date : 2024-05-01 DOI: 10.1016/j.matre.2024.100272
Tianyun Zhang , Xiaohong Shi , Yu Li , Sambasivam Sangaraju , Fujuan Wang , Liang Yang , Fen Ran

Aqueous zinc metal batteries are regarded as the most promising energy storage system due to their advantages of high safety, low cost, and high theoretical capacity. However, the growth of dendrites and the occurrence of side reactions hinder the development of zinc metal batteries. Despite previous attempts to design advanced hydrogel electrolytes, achieving high mechanical performance and ionic conductivity of hydrogel electrolytes has remained challenging. In this work, a hydrogel electrolyte with an ionic crosslinked network is prepared by carboxylic bacterial cellulose fiber and imidazole-type ionic liquid, following by a covalent network of polyacrylamide. The hydrogel electrolyte possesses a superior ionic conductivity of 43.76 mS cm−1, leading to a Zn2+ migration number of 0.45, and high mechanical performance with an elastic modulus of 3.48 GPa and an elongation at breaking of 38.36%. More importantly, under the anion-coordination effect of the carboxyl group in bacterial cellulose and [BF4] in imidazole-type ionic liquid, the solvation sheath of hydrated Zn2+ ions and the nucleation overpotential of Zn plating are regulated. The results of cycled testing show that the growth of zinc dendrites is effectively inhibited and the generation of irreversible by-products is reduced. With the carboxylic bacterial cellulose-based hydrogel electrolyte, the Zn||Zn symmetric batteries offer good cyclability as well as Zn||Ti batteries.

锌金属水电池具有安全性高、成本低和理论容量大等优点,被认为是最有前途的储能系统。然而,枝晶的生长和副反应的发生阻碍了锌金属电池的发展。尽管以前曾尝试过设计先进的水凝胶电解质,但实现水凝胶电解质的高机械性能和离子导电性仍然具有挑战性。在这项研究中,利用羧基细菌纤维素纤维和咪唑类离子液体以及聚丙烯酰胺共价网络制备了一种具有离子交联网络的水凝胶电解质。该水凝胶电解质具有 43.76 mS cm-1 的优异离子电导率,使 Zn2+ 迁移数达到 0.45,并具有 3.48 GPa 的弹性模量和 38.36% 的断裂伸长率等高机械性能。更重要的是,在细菌纤维素中的羧基和咪唑类离子液体中的[BF4]-阴离子配位作用下,水合 Zn2+ 离子的溶解鞘和 Zn 镀层的成核过电位得到了调节。循环测试结果表明,锌树枝状突起的生长得到了有效抑制,不可逆副产物的生成也有所减少。在羧酸菌纤维素水凝胶电解质的作用下,Zn||Zn 对称电池与 Zn||Ti 电池一样具有良好的循环性能。
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引用次数: 0
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材料导报:能源(英文)
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