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Morphology-controlled synthesis of multi-metal-based spinel oxide nanocatalysts and their performance for oxygen reduction 多金属基尖晶石氧化物纳米催化剂的形态控制合成及其氧气还原性能
Pub Date : 2024-08-22 DOI: 10.1002/elt2.62
Can Li, Jinfong Pan, Xiaobo Chen, Lihua Zhang, Anna Dennett, Prabhu Bharathan, Douglas Lee, Guangwen Zhou, Jiye Fang

We present a one-pot colloidal synthesis method for producing monodisperse multi-metal (Co, Mn, and Fe) spinel nanocrystals (NCs), including nanocubes, nano-octahedra, and concave nanocubes. This study explores the mechanism of morphology control, showcasing the pivotal roles of metal precursors and capping ligands in determining the exposed crystal planes on the NC surface. The cubic spinel NCs, terminated with exclusive {100}-facets, demonstrate superior electrocatalytic activity for the oxygen reduction reaction (ORR) in alkaline media compared to their octahedral and concave cubic counterparts. Specifically, at 0.85 V, (CoMn)Fe2O4 spinel oxide nanocubes achieve a high mass activity of 23.9 A/g and exhibit excellent stability, highlighting the promising ORR performance associated with {100}-facets of multi-metal spinel oxides over other low-index and high-index facets. Motivated by exploring the correlation between ORR performance and surface atom arrangement (active sites), surface element composition, as well as other factors, this study introduces a prospective approach for shape-controlled synthesis of advanced spinel oxide NCs. It underscores the significance of catalyst shape control and suggests potential applications as nonprecious metal ORR electrocatalysts.

我们提出了一种一锅胶体合成法,用于生产单分散多金属(钴、锰和铁)尖晶石纳米晶体(NC),包括纳米立方体、纳米八面体和凹面纳米立方体。本研究探讨了形态控制机制,展示了金属前驱体和封接配体在决定 NC 表面裸露晶面方面的关键作用。与八面体和凹立方对应物相比,以独有的{100}面终止的立方尖晶石 NC 在碱性介质中的氧还原反应(ORR)中表现出更高的电催化活性。具体而言,在 0.85 V 的电压下,(CoMn)Fe2O4 尖晶石氧化物纳米立方体的质量活性高达 23.9 A/g,并表现出卓越的稳定性,这突出表明与其他低指数和高指数面相比,多金属尖晶石氧化物的{100}面具有良好的氧还原反应性能。通过探索 ORR 性能与表面原子排列(活性位点)、表面元素组成以及其他因素之间的相关性,本研究介绍了一种先进尖晶石氧化物 NC 形状控制合成的前瞻性方法。它强调了催化剂形状控制的重要性,并提出了作为非贵金属 ORR 电催化剂的潜在应用。
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引用次数: 0
Electrocatalytic upcycling of plastic waste: Progress, challenges, and future 塑料废物的电催化升级再循环:进展、挑战和未来
Pub Date : 2024-08-21 DOI: 10.1002/elt2.63
Jinzhou Li, Junliang Chen, Luyao Zhang, Juan Matos, Li Wang, Jianping Yang

The escalating accumulation of plastic waste has been developed into a formidable global environmental challenge. Traditional disposal methods such as landfilling and incineration not only exacerbate environmental degradation by releasing harmful chemicals and greenhouse gases, but also squander finite resources that could otherwise be recycled or repurposed. Upcycling is a kind of plastic recycling technology that converts plastic waste into high-value chemicals and helps to avoid resource waste and environmental pollution. Electrocatalytic upcycling emerges as a novel technology distinguished by its mild operational conditions, high transformation efficiency and product selectivity. This review commences with an overview of the recycling and upcycling technology employed in plastic waste management and the respective advantages and inherent limitations are also delineated. The different types of plastic waste upcycled by electrocatalytic strategy are then discussed and the plastic waste transformation process is examined together with the mechanisms underlying the electrocatalytic upcycling. Furthermore, the structure-activity relationships between electrocatalysts and plastic waste upcycling performance are also elucidated. The review aims to furnish readers with a comprehensive understanding of the electrocatalytic techniques for plastic waste upcycling and to provide a guidance for the design of electrocatalysts towards efficient plastic waste transformation.

塑料废物的不断累积已发展成为一项严峻的全球环境挑战。填埋和焚烧等传统处理方式不仅会释放有害化学物质和温室气体,加剧环境恶化,还会浪费原本可以回收利用的有限资源。升级再造是一种塑料回收技术,可将塑料废弃物转化为高价值的化学品,有助于避免资源浪费和环境污染。电催化升 级再循环是一种新型技术,具有操作条件温和、转化效率高和产品选择性强等特点。本综述首先概述了塑料废物管理中采用的回收和升级再循环技术,并对其各自的优势和固有的局限性进行了阐述。然后,讨论了通过电催化策略进行升级再循环的不同类型的塑料废物,并研究了塑料废物的转化过程以及电催化升级再循环的内在机制。此外,还阐明了电催化剂与塑料废物循环利用性能之间的结构-活性关系。本综述旨在让读者全面了解塑料废弃物升级再循环的电催化技术,并为设计高效塑料废弃物转化的电催化剂提供指导。
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引用次数: 0
Phase-controllable cobalt phosphide heterostructure for efficient electrocatalytic hydrogen evolution in water and seawater 用于水和海水中高效电催化氢进化的相位可控磷化钴异质结构
Pub Date : 2024-07-25 DOI: 10.1002/elt2.58
Guo Huang, Yujin Huang, Asad Ali, Zhijie Chen, Pei Kang Shen, Bing-Jie Ni, Jinliang Zhu

Cobalt phosphides attract broad attention as alternatives to platinum-based materials towards hydrogen evolution reaction (HER). The catalytic performance of cobalt phosphides largely depends on the phase structure, but figuring out the optimal phase towards HER remains challenging due to their diverse stoichiometries. In our work, a series of cobalt phosphide nanoparticles with different phase structures but similar particle sizes (CoP-Co2P, Co2P-Co, Co2P, and CoP) on a porous carbon network (PC) were accurately synthesized. The CoP-Co2P/PC heterostructure demonstrates upgraded HER catalytic activity with a low overpotential of 96.7 and 162.1 mV at 10 mA cm−2 in 1 M KOH and 1 M phosphate-buffered saline solution, respectively, with a long-term (120 h) durability. In addition, the CoP-Co2P/PC exhibits good HER performance in alkaline seawater, with a small overpotential of 111.2 mV at 10 mA cm−2 and a low Tafel slope of 64.2 mV dec−1, as well as promising stability. Density functional theory results show that the Co2P side of the CoP-Co2P/PC heterostructure has the best Gibbs free energy of each step for HER, which contributes to the high HER activity. This study sets the stage for the advancement of high-performance HER electrocatalysts and the implementation of large-scale seawater electrolysis.

磷化钴作为铂基材料的替代品,在氢进化反应(HER)中备受关注。磷化钴的催化性能在很大程度上取决于相结构,但由于磷化钴的化学计量学各不相同,因此找出氢进化反应的最佳相仍然具有挑战性。在我们的工作中,我们在多孔碳网络(PC)上精确合成了一系列具有不同相结构但粒径相似的磷化钴纳米颗粒(CoP-Co2P、Co2P-Co、Co2P 和 CoP)。CoP-Co2P/PC 异质结构表现出更高的 HER 催化活性,在 1 M KOH 和 1 M 磷酸盐缓冲盐溶液中,10 mA cm-2 的过电位分别为 96.7 和 162.1 mV,且具有长期(120 h)的耐久性。此外,CoP-Co2P/PC 在碱性海水中表现出良好的 HER 性能,在 10 mA cm-2 时过电位小(111.2 mV),塔菲尔斜率低(64.2 mV dec-1),并且具有良好的稳定性。密度泛函理论结果表明,CoP-Co2P/PC 异质结构的 Co2P 侧在 HER 的每个步骤中都具有最佳的吉布斯自由能,这有助于提高 HER 活性。这项研究为开发高性能 HER 电催化剂和实现大规模海水电解奠定了基础。
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引用次数: 0
Perspective on eutectic electrolytes for next-generation batteries 下一代电池共晶电解质展望
Pub Date : 2024-07-11 DOI: 10.1002/elt2.57
Jiajie Zhang, Yonghui Zhang, Jie Fu, Xianfeng Li, Changkun Zhang

The environmental challenges and growing energy demand have promoted the development of renewable energy, including solar, tidal, and wind. The next-generation electrochemical energy storage (EES), incorporating flow battery (FB) and metal-based battery (MB, Li, Na, Zn, Mg, etc.) received more attention. The flammable electrolytes in nonaqueous batteries have raised serious safety hazards and more unconventional electrolyte systems have been proposed recently. An emerging class of electrolytes, eutectic electrolytes have been reported in many batteries due to the facile preparation, concentrated states, and unique ion transport properties. In FB, eutectic electrolytes can significantly increase the energy density by promoting the molar ratio of redox active materials. In MB, eutectic electrolytes reduce the vapor pressure and toxicity, inhibit metal dendrites growth, and enlarge the electrochemical window. In this review, we summarize the progress status of different eutectic electrolytes on both FBs and MBs. We expect this review can supply the guidance for the application of eutectic electrolytes in EES.

环境挑战和日益增长的能源需求促进了太阳能、潮汐能和风能等可再生能源的发展。下一代电化学储能(EES),包括液流电池(FB)和金属基电池(MB、Li、Na、Zn、Mg 等)受到更多关注。非水性电池中的易燃电解质存在严重的安全隐患,因此最近提出了更多的非常规电解质系统。共晶电解质是一类新兴的电解质,由于其易于制备、具有浓缩状态和独特的离子传输特性,在许多电池中都有应用。在 FB 中,共晶电解质可以通过提高氧化还原活性材料的摩尔比来显著提高能量密度。在 MB 中,共晶电解质可降低蒸气压和毒性,抑制金属枝晶的生长,扩大电化学窗口。在本综述中,我们总结了不同共晶电解质在 FB 和 MB 中的应用进展情况。我们希望本综述能为共晶电解质在 EES 中的应用提供指导。
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引用次数: 0
MOF-derived Co/C-anchored MoS2-based phase change materials toward thermal management and microwave absorption 基于 MOF 衍生 Co/C-anchored MoS2 的相变材料,用于热管理和微波吸收
Pub Date : 2024-07-03 DOI: 10.1002/elt2.56
Yang Li, Xukang Han, Jiaying Zhu, Yuhao Feng, Panpan Liu, Xiao Chen

With the miniaturization and integration of electronic devices, developing advanced multifunctional phase change materials (PCMs) integrating thermal storage, thermal conduction, and microwave absorption to address electromagnetic interference, thermal dissipation, and instantaneous thermal shock is imperative. Herein, we proposed an extensible strategy to synthesize MOF-derived Co/C-anchored MoS2-based PCMs using high-temperature carbonation of flower-like MoS2 grown in situ by ZIF67 and vacuum impregnation of paraffin. The resulting MoS2@Co/C-paraffin composite PCMs exhibited good thermal storage density, thermal cycling stability, and long-term durability. The thermal conductivity of composite PCMs was 44% higher than that of pristine paraffin due to the construction of low interfacial thermal resistance. More attractively, our designed composite PCMs also possessed −57.15 dB minimum reflection loss at 9.2 GHz with a thickness of 3.0 mm, corresponding to an effective absorption bandwidth of 3.86 GHz. The excellent microwave absorption was attributed to the multicomponent synergy of magnetic loss from Co nanoparticles and conductive loss from MOF-derived carbon layers, and multiple reflection of MoS2 nanowrinkle, along with good impedance matching. This study provided a meaningful reference for the widespread application of composite PCMs combining thermal storage, thermal conduction, and microwave absorption in high-power miniaturized electronic devices.

随着电子设备的微型化和集成化,开发集蓄热、热传导和微波吸收于一体的先进多功能相变材料 (PCM) 以解决电磁干扰、热耗散和瞬时热冲击问题势在必行。在此,我们提出了一种可扩展的策略,利用 ZIF67 对原位生长的花状 MoS2 进行高温碳化和石蜡真空浸渍,合成 MOF 衍生的 Co/C-anchored MoS2 基 PCM。所制备的 MoS2@Co/C-paraffin 复合 PCM 具有良好的蓄热密度、热循环稳定性和长期耐久性。由于构建了低界面热阻,复合 PCM 的热导率比原始石蜡高 44%。更吸引人的是,我们设计的复合 PCM 在 9.2 GHz 频率下具有 -57.15 dB 的最小反射损耗,厚度为 3.0 mm,有效吸收带宽为 3.86 GHz。优异的微波吸收性能归功于 Co 纳米粒子的磁性损耗、MOF 衍生碳层的导电损耗、MoS2 纳米皱纹的多重反射以及良好的阻抗匹配等多组分协同作用。这项研究为集热存储、热传导和微波吸收于一体的复合 PCM 在大功率微型电子设备中的广泛应用提供了有意义的参考。
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引用次数: 0
Multifunctional diamond-based catalysts: Promising candidates for energy conversions in extreme environments—A mini-review 多功能金刚石催化剂:在极端环境中进行能量转换的理想候选者--微型综述
Pub Date : 2024-07-01 DOI: 10.1002/elt2.45
Ziwei Zhao, Xiaowu Gao, Hansong Zhang, Keran Jiao, Pengfei Song, Yumin Zhang, Yongjie Wang, Jiaqi Zhu

In order to properly utilize the abundant CO2 and water resources, various catalytic materials have been developed to convert them into valuable chemicals as renewable fuels electrochemically or photochemically. Currently, most studies are conducted under mild laboratory conditions, but for some extreme environments, such as Mars and space stations, there is an urgent need to develop new catalysts satisfying such special requirements. Conventional catalytic materials mainly focus on metals and narrow bandgap semiconductor materials, while the research on wide and ultrawide bandgap materials that can inherently withstand extreme conditions has not received enough attention. Given the robust stability and excellent physico-chemical properties of diamond, it can be expected to perform in harsh environments for electrocatalysis or photocatalysis that has not been investigated thoroughly. Here, this review summarizes the catalytic functionality of diamond-based electrodes with various but tunable product selectivity to obtain the varied C1 or C2+ products, and discusses some important factors playing a key role in manipulating the catalytic activity. Moreover, the unique solvation electron effect of diamond gives it a significant advantage in photocatalytic conversions which is also summarized in this mini-review. In the end, prospects are made for the application of diamond-based catalysts under various extreme conditions. The challenges that may be faced in practical applications are also summarized and future breakthrough directions are proposed at the end.

为了合理利用丰富的二氧化碳和水资源,人们开发了各种催化材料,通过电化学或光化学方法将其转化为有价值的化学品,作为可再生燃料。目前,大多数研究都是在温和的实验室条件下进行的,但对于一些极端环境,如火星和空间站,迫切需要开发新的催化剂来满足这些特殊要求。传统的催化材料主要集中在金属和窄带隙半导体材料上,而本身就能承受极端条件的宽带隙和超宽带隙材料的研究还没有得到足够的重视。鉴于金刚石具有强大的稳定性和优异的物理化学特性,它有望在恶劣环境中发挥电催化或光催化的作用,但这方面的研究还不够深入。本综述总结了金刚石电极的催化功能,它具有多种可调的产物选择性,可获得不同的 C1 或 C2+ 产物,并讨论了在操纵催化活性过程中起关键作用的一些重要因素。此外,金刚石独特的溶解电子效应使其在光催化转化方面具有显著优势,本微型综述也对此进行了总结。最后,还展望了金刚石催化剂在各种极端条件下的应用前景。最后还总结了实际应用中可能面临的挑战,并提出了未来的突破方向。
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引用次数: 0
Directing the photogenerated charge flow in a photocathodic metal protection system with single-domain ferroelectric PbTiO3 nanoplates 利用单域铁电 PbTiO3 纳米板引导光阴极金属保护系统中的光生电荷流
Pub Date : 2024-06-26 DOI: 10.1002/elt2.51
Hui Xie, Jianyou Yu, Yuchen Fang, Zhijun Wang, Shihe Yang, Zheng Xing

Photocathodic protection (PCP) is arguably an ideal alternative technology to the conventional electrochemical cathodic protection methods for corrosion mitigation of metallic infrastructure due to its eco-friendliness and low-energy-consumption, but the construction of highly-efficient PCP systems still remains challenging, caused primarily by the lack of driving force to guide the charge flow through the whole PCP photoanodes. Here, we tackle this key issue by equipping the PCP photoanode with ferroelectric single-domain PbTiO3 nanoplates, which can form a directional “macroscopic electric field” throughout the entire photoanode controllable by external polarization. The properly poled PCP photoanode allows the photogenerated electrons and holes to migrate in opposite directions, that is, electrons to the protected metal and holes to the photoanode/electrolyte interface, leading to largely suppressed charge annihilation and consequently a considerable boost in the overall solar energy conversion efficiency of the PCP system. The as-fabricated photoanode can not only supply sufficient photocurrent to 304 stainless steel to initiate cathodic protection, but also shift the metal potential to the corrosion-free range. Our findings provide a viable design strategy for future high-performance PCP systems based on ferroelectric nanomaterials with enhanced charge flow manipulation.

光电阴极保护(PCP)因其生态友好性和低能耗,可以说是金属基础设施腐蚀缓解领域传统电化学阴极保护方法的理想替代技术,但高效 PCP 系统的构建仍面临挑战,主要原因是缺乏引导电荷流经整个 PCP 光阳极的驱动力。在这里,我们通过在 PCP 光阳极中加入铁电单域 PbTiO3 纳米板来解决这一关键问题,这种纳米板可以在整个光阳极中形成定向的 "宏观电场",并可通过外部极化进行控制。经过适当极化的 PCP 光阳极允许光生电子和空穴向相反的方向迁移,即电子迁移到受保护的金属,空穴迁移到光阳极/电解质界面,从而在很大程度上抑制了电荷湮灭,从而大大提高了 PCP 系统的整体太阳能转换效率。制作完成的光阳极不仅能为 304 不锈钢提供足够的光电流以启动阴极保护,还能将金属电位转移到无腐蚀范围。我们的研究结果为未来基于铁电纳米材料的高性能 PCP 系统提供了一种可行的设计策略,该系统具有更强的电荷流操控能力。
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引用次数: 0
Dual function of formamidinium chloride additive improves the efficiency and stability of low-dimensional perovskite solar cells 甲脒氯化物添加剂的双重功能提高了低维过氧化物太阳能电池的效率和稳定性
Pub Date : 2024-06-16 DOI: 10.1002/elt2.52
Lvpeng Yang, Tong Bie, Peiyu Ma, Jin Xin, Tho D. Nguyen, Ming Shao

Despite their excellent intrinsic stability, low-dimensional Ruddlesden-Popper (LDRP) perovskites face challenges with low power conversion efficiency (PCE), primarily due to the widen bandgap and limited charge transport caused by the bulky spacer cation. Herein, we introduce formamidinium chloride (FACl) as an additive into (4-FPEA)2MA4Pb5I16 perovskite. On the one hand, the addition of FACl narrows the bandgap through cation exchange between MA+ and FA+, thereby extending the light absorption range and enhancing photocurrent generation. On the other hand, this MA+/FA+ cation exchange decelerates the sublimation of methylammonium chloride and prolongs the crystallization of LDRP perovskite, leading to higher crystallinity and better film quality with a decreased trap-state density. Consequently, this approach led to a remarkable PCE of 20.46% for <n> = 5 LDRP perovskite solar cells (PSCs), ranking among the highest for MA/FA mixed low dimensional PSCs reported to date. Remarkably, our PSCs maintained 90% and 92% of the initial efficiency even after 1300 h at (60 ± 5)°C and (60 ± 5)% relative humidity, respectively. This work promotes the development of LDRP PSCs with excellent efficiency and environmental stability for potential commercial application.

尽管低维 Ruddlesden-Popper(LDRP)包晶石具有出色的内在稳定性,但却面临着功率转换效率(PCE)低的挑战,这主要是由于笨重的间隔阳离子导致带隙变宽和电荷传输受限。在此,我们在 (4-FPEA)2MA4Pb5I16 包晶中引入了甲脒氯化物(FACl)作为添加剂。一方面,FACl 的加入通过 MA+ 和 FA+ 之间的阳离子交换缩小了带隙,从而扩大了光吸收范围并增强了光电流的产生。另一方面,MA+/FA+ 阳离子交换可减缓甲基氯化铵的升华,延长 LDRP 包晶体的结晶时间,从而提高结晶度,改善薄膜质量,降低陷阱态密度。因此,这种方法使 <n> = 5 LDRP 包晶体太阳能电池(PSCs)的 PCE 达到了 20.46%,是迄今为止报告的 MA/FA 混合低维 PSCs 中最高的。值得注意的是,即使在(60±5)℃和(60±5)%相对湿度条件下放置 1300 小时后,我们的 PSC 仍分别保持了 90% 和 92% 的初始效率。这项工作推动了具有卓越效率和环境稳定性的 LDRP PSCs 的发展,为其潜在的商业应用提供了可能。
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引用次数: 0
The importance of precise and suitable descriptors in data-driven approach to boost development of lithium batteries: A perspective 数据驱动法中精确、合适的描述符对促进锂电池开发的重要性:透视
Pub Date : 2024-06-02 DOI: 10.1002/elt2.41
Zehua Wang, Li Wang, Hao Zhang, Hong Xu, Xiangming He

Conventional approaches for developing new materials may no longer be adequate to meet the urgent needs of humanity's energy transition. The emergence of machine learning (ML) and artificial intelligence (AI) has led materials scientists to recognize the potential of using AI/ML to accelerate the creation of new battery materials. Although fixed material properties have been extensively studied as descriptors to establish the link between AI and materials chemistry, they often lack versatility and accuracy due to a lack of understanding of the underlying mechanisms of AI/ML. Therefore, materials scientists need to have a comprehensive understanding of the operational mechanisms and learning logic of AI/ML to design more accurate descriptors. This paper provides a review of previous research studies conducted on AI, ML, and descriptors, which have been used to address challenges at various levels, ranging from materials development to battery performance prediction. Additionally, it introduces the basics of AI and ML to assist materials and battery developers in comprehending their operational mechanisms. The paper demonstrates the significance of precise and suitable ML descriptors in the creation of new battery materials. It does so by providing examples, summarizing current descriptors and ML algorithms, and examining the potential implications of future AI advancements for the sustainable energy industry.

开发新材料的传统方法可能已无法满足人类能源转型的迫切需求。机器学习(ML)和人工智能(AI)的出现使材料科学家认识到利用 AI/ML 加速创造新型电池材料的潜力。虽然固定的材料属性已被广泛研究,作为建立人工智能与材料化学之间联系的描述符,但由于缺乏对人工智能/ML 潜在机制的了解,这些属性往往缺乏通用性和准确性。因此,材料科学家需要全面了解人工智能/ML 的运行机制和学习逻辑,以设计出更精确的描述符。本文回顾了以往关于人工智能、ML 和描述符的研究,这些研究已被用于应对从材料开发到电池性能预测等不同层面的挑战。此外,论文还介绍了人工智能和 ML 的基础知识,以帮助材料和电池开发人员理解其运行机制。本文展示了精确、合适的 ML 描述符对创造新型电池材料的重要意义。本文通过举例说明、总结当前的描述符和 ML 算法,以及研究未来人工智能进步对可持续能源行业的潜在影响来实现这一目的。
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引用次数: 0
Cover Image, Volume 2, Number 2, May 2024 封面图片,第 2 卷第 2 号,2024 年 5 月
Pub Date : 2024-05-30 DOI: 10.1002/elt2.54
Gaihong Wang, Zhijie Chen, Wei Wei, Bing-Jie Ni

Electro-upcycling of plastic provides a new avenue for sustainable plastic waste management and fuel/chemical production in a low-carbon manner. In this review (DOI: 10.1002/elt2.34), we comprehensively examine recent advances in the development of plastic waste electro-upcycling. Key electrooxidation reactions involved in the electrochemical conversion of diverse plastic waste, advanced integrated electrolysis systems, and efficient electrocatalyst design strategies are fully discussed. We also analyze perspectives for guiding further study in this emerging field.

塑料电循环利用为可持续塑料废物管理和低碳燃料/化学品生产提供了一条新途径。在这篇综述(DOI: 10.1002/elt2.34)中,我们全面探讨了塑料废物电升级循环利用的最新进展。文中充分讨论了各种塑料废弃物电化学转化过程中涉及的关键电氧化反应、先进的集成电解系统以及高效电催化剂的设计策略。我们还分析了指导这一新兴领域进一步研究的前景。
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引用次数: 0
期刊
Electron
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