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Advances in electrocatalytic urea synthesis: From fundamentals to applications 电催化尿素合成的进展:从基础到应用
Pub Date : 2024-10-05 DOI: 10.1016/j.apmate.2024.100245
Zhenlin Mo, Jincheng Mu, Baojun Liu
The electrocatalytic synthesis of urea (ESU) is a green and sustainable alternative to conventional production methods, and the related research is still in its infancy. Up to now, the field has been explored by several reviews, however, the authors are focusing on some particular problems and could not provide a holistic view of the ESU. Based on these considerations, the novelty of this review lies in its comprehensive and systematic framework, as well as its in-depth analysis and general summary of several key issues. Hence, in this review, we critically evaluated the ESU through in-depth studies of various aspects, including nitrogen sources, catalysts choice, conditions modifications, detection methods, product calculations, and mechanisms evaluation, etc. In addition, after analyzing the reaction routes, reaction kinetics/thermodynamics and techno-economics assessment are also investigated. Finally, the summary and outlook are presented eventually, providing valuable insights for the related research. We believe that we will provide researchers with a comprehensive and clear picture of green synthesized urea, which is of great academic and practical significance.
电催化合成尿素(ESU)是一种替代传统生产方法的绿色、可持续的方法,相关研究仍处于起步阶段。迄今为止,已有多篇综述对该领域进行了探讨,但作者们关注的都是一些特定的问题,无法对 ESU 提供一个整体的视角。基于上述考虑,本综述的新颖之处在于其全面、系统的框架,以及对几个关键问题的深入分析和概括总结。因此,在本综述中,我们通过对氮源、催化剂选择、条件修改、检测方法、产物计算和机理评估等各个方面的深入研究,对 ESU 进行了严格的评估。此外,在分析反应路线后,还研究了反应动力学/热力学和技术经济学评估。最后,我们进行了总结和展望,为相关研究提供了有价值的启示。我们相信,我们将为研究人员提供一个全面而清晰的绿色合成尿素的全貌,具有重要的学术和实践意义。
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引用次数: 0
Heteroatom doping in 2D MXenes for energy storage/conversion applications 在二维二氧杂环烯中掺杂杂原子以实现能量存储/转换应用
Pub Date : 2024-10-05 DOI: 10.1016/j.apmate.2024.100246
Sumanta Sahoo , Rajesh Kumar , Iftikhar Hussain , Kaili Zhang
MXenes (inorganic metal carbides, nitrides, and carbonitrides) are currently the rising star of two-dimensional (2D) family. After its discovery in 2011, initial research was concentrated on pristine MXenes only. However, in the last few years, the MXene family has been expanded with the exploration of novel double MXenes, synthesis of non-Ti MXenes, and heteroatom doping of MXenes. The current review article delivers an exclusive overview of the current research trends on the heteroatom doping of MXenes. The recent advances in heteroatom doping of MXenes (majorly Ti-MXenes) for energy storage/conversion applications including secondary batteries (Li-ion, Li–S, Na–S, Na-ion, K-ion, Zn-ion batteries), supercapacitors, electrocatalysis, etc. are summarized. A brief overview of the defects as well as doping in various 2D materials is included in the manuscript. Various doping strategies of MXenes are outlined. Moreover, the impact of artificial intelligence/machine learning on MXene research is also concisely discussed. Additionally, the advantages of doping on MXenes are discussed in detail. Lastly, the existing challenges and future prospects of doped MXenes are addressed. It is expected that the current review will open new prospects for the fabrication of advanced energy devices through heteroatom doping of MXenes.
MXenes(无机金属碳化物、氮化物和碳氮化物)是目前二维(2D)家族中一颗冉冉升起的新星。在 2011 年被发现后,最初的研究只集中在原始的 MXenes 上。然而,在过去的几年中,随着对新型双 MXenes、非钛 MXenes 的合成以及 MXenes 的杂原子掺杂的探索,MXene 家族得到了扩展。本综述文章独家概述了当前有关掺杂杂原子的 MXenes 的研究趋势。文章概述了掺杂杂原子的二氧化二烯(主要是钛-二氧化二烯)在能量存储/转换应用方面的最新进展,包括二次电池(锂离子电池、锂-S 电池、Na-S 电池、Na-离子电池、K-离子电池、Zn-离子电池)、超级电容器、电催化等。手稿中还简要概述了各种二维材料的缺陷和掺杂情况。概述了 MXenes 的各种掺杂策略。此外,还简明扼要地讨论了人工智能/机器学习对 MXene 研究的影响。此外,还详细讨论了掺杂 MXenes 的优势。最后,探讨了掺杂 MXenes 的现有挑战和未来前景。预计本综述将为通过掺杂二氧化二烯的杂原子制造先进能源设备开辟新的前景。
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引用次数: 0
Atomically dispersed NiOx cluster on high-index Pt facets boost ethanol electrooxidation through long-range synergistic sites 高指数铂表面上的原子分散氧化镍团簇通过长程协同位点促进乙醇电氧化作用
Pub Date : 2024-09-30 DOI: 10.1016/j.apmate.2024.100244
Yao Wang , Meng Zheng , Yunrui Li , Lidan Zhu , Haoran Li , Qishun Wang , Hui Zhao , Jiawei Zhang , Yuming Dong , Yongfa Zhu
Constructing the desired long-range dual sites to enhance the C–C bond-cleavage and CO-tolerate ability during ethanol oxidation reaction is of importance for further applications. Herein, the concept of holding atomically dispersed NiOx cluster supported on Pt-based high-index facets (NiOx/Pt) is proposed to build O-bridged Pt–Ni dual sites. Strikingly, the obtained NiOx/Pt dual sites show 4.97 times specific activity higher than that of commercial Pt/C (0.35 ​mA ​cm−2), as well as outstanding CO-tolerance and durability. The advanced electrochemical in-situ characterizations reveal that the NiOx/Pt can accelerate rapid dehydroxylation and C–C bond-cleavage over the Pt–Ni dual sites. Theoretical calculations disclose that the atomically dispersed NiOx species can lower the adsorption/reaction energy barriers of intermediates. This tactic provides a promising methodology on regulating the surface synergistic sites via engineering atomically dispersed oxide site.
在乙醇氧化反应过程中,构建所需的长程双位点以增强 C-C 键的清除能力和 CO 的溶解能力对进一步的应用具有重要意义。本文提出了在铂基高指数面(NiOx/Pt)上支撑原子分散的 NiOx 簇的概念,以构建 O 桥接的铂镍双位点。引人注目的是,所获得的 NiOx/Pt 双基点的比活度是商用 Pt/C 的 4.97 倍(0.35 mA cm-2),而且具有出色的一氧化碳耐受性和耐久性。先进的电化学原位表征显示,NiOx/Pt 比 Pt-Ni 双位点更能加速脱羟基和 C-C 键的裂解。理论计算表明,原子分散的氧化镍物种可以降低中间产物的吸附/反应能垒。这种方法为通过设计原子分散氧化物位点来调节表面协同位点提供了一种可行的方法。
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引用次数: 0
Green and regulable synthesis of CdNCN on CdS semiconductor: Atomic-level heterostructures for enhanced photocatalytic hydrogen evolution 在 CdS 半导体上绿色可控地合成 CdNCN:用于增强光催化氢进化的原子级异质结构
Pub Date : 2024-09-26 DOI: 10.1016/j.apmate.2024.100242
Taiyu Huang , Zimo Huang , Xixian Yang , Siyuan Yang , Qiongzhi Gao , Xin Cai , Yingju Liu , Yueping Fang , Shanqing Zhang , Shengsen Zhang
In the realm of photoenergy conversion, the scarcity of efficient light-driven semiconductors poses a significant obstacle to the advancement of photocatalysis, highlighting the critical need for researchers to explore novel semiconductor materials. Herein, we present the inaugural synthesis of a novel semiconductor, CdNCN, under mild conditions, while shedding light on its formation mechanism. By effectively harnessing the [NCN]2 moiety in the thiourea process, we successfully achieve the one-pot synthesis of CdNCN-CdS heterostructure photocatalysts. Notably, the optimal CdNCN-CdS sample demonstrates a hydrogen evolution rate of 14.7 ​mmol ​g−1 ​h−1 under visible light irradiation, establishing itself as the most efficient catalyst among all reported CdS-based composites without any cocatalysts. This outstanding hydrogen evolution performance of CdNCN-CdS primarily arises from two key factors: i) the establishment of an atomic-level N-Cd-S heterostructure at the interface between CdNCN and CdS, which facilitating highly efficient electron transfer; ii) the directed transfer of electrons to the (110) crystal plane of CdNCN, promoting optimal hydrogen adsorption and active participation in the hydrogen evolution reaction. This study provides a new method for synthesizing CdNCN materials and offers insights into the design and preparation of innovative atomic-level composite semiconductor photocatalysts.
在光能转换领域,高效光驱动半导体的稀缺性严重阻碍了光催化技术的发展,凸显了研究人员探索新型半导体材料的迫切需要。在此,我们首次在温和条件下合成了一种新型半导体--CdNCN,同时揭示了其形成机理。通过有效利用硫脲工艺中的[NCN]2-分子,我们成功地实现了 CdNCN-CdS 异质结构光催化剂的一锅合成。值得注意的是,最佳的 CdNCN-CdS 样品在可见光照射下的氢气进化速率为 14.7 mmol g-1 h-1,在所有已报道的不含任何助催化剂的 CdS 基复合材料中成为最高效的催化剂。CdNCN-CdS 优异的氢演化性能主要源于两个关键因素:i) 在 CdNCN 和 CdS 的界面上建立了原子级的 N-Cd-S 异质结构,促进了高效的电子转移;ii) 电子定向转移到 CdNCN 的(110)晶面上,促进了最佳的氢吸附并积极参与氢演化反应。这项研究提供了一种合成 CdNCN 材料的新方法,并为设计和制备创新的原子级复合半导体光催化剂提供了启示。
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引用次数: 0
Atmosphere engineering of metal-free Te/C3N4 p-n heterojunction for nearly 100% photocatalytic converting CO2 to CO 无金属 Te/C3N4 p-n 异质结的大气工程,几乎 100% 光催化将 CO2 转化为 CO
Pub Date : 2024-09-26 DOI: 10.1016/j.apmate.2024.100243
Huange Liao , Kai Huang , Weidong Hou , Huazhang Guo , Cheng Lian , Jiye Zhang , Zheng Liu , Liang Wang
Carbon nitride (CN)-based heterojunction photocatalysts hold promise for efficient carbon dioxide (CO2) reduction. However, suboptimal production yields and limited selectivity in CO2 conversion pose significant barriers to achieving efficient CO2 conversion. Here, we present the construction of a p-n heterojunction between ultrasmall Te NPs and CN nanosheet using a novel tandem hydrothermal-calcination synthesis strategy. Through ammonia-assisted calcination, ultrasmall Te NPs are grown in-situ on the CN nanosheets’ surface, resulting in the generation of a robust p-n heterojunction. The synthesized heterojunction exhibits increased specific surface area, reinforced visible light absorption, intensive CO2 adsorption capacity, and efficient charge transfer. The optimum Te/CN-NH3 demonstrates superior photocatalytic CO2 reduction activity and durability, with nearly 100 ​% selectivity for CO and a yield as high as 92.0 ​μmol ​g−1 ​h−1, a fourfold increase compared to pure CN. Experimental and theoretical calculations unravel that the strong built-in electric field of the Te/CN-NH3 p-n heterojunction accelerates the migration of photogenerated electrons from Te NPs to the N site on CN nanosheets, thereby promoting CO2 reduction. This study provides a promising material design approach for the construction of high-performance p-n heterojunction photocatalysts.
基于氮化碳(CN)的异质结光催化剂有望实现二氧化碳(CO2)的高效还原。然而,二氧化碳转化过程中不理想的产量和有限的选择性是实现二氧化碳高效转化的重大障碍。在此,我们采用一种新颖的串联水热-煅烧合成策略,构建了超小 Te NPs 与 CN 纳米片之间的 p-n 异质结。通过氨辅助煅烧,超小 Te NPs 在 CN 纳米片表面原位生长,从而生成了一个坚固的 p-n 异质结。合成的异质结具有更高的比表面积、更强的可见光吸收能力、更强的二氧化碳吸附能力以及高效的电荷转移能力。最佳的 Te/CN-NH3 显示出卓越的光催化二氧化碳还原活性和耐久性,对一氧化碳的选择性接近 100%,产率高达 92.0 μmol g-1 h-1,比纯 CN 提高了四倍。实验和理论计算表明,Te/CN-NH3 p-n 异质结的强内置电场加速了光生电子从 Te NPs 迁移到 CN 纳米片上的 N 位点,从而促进了 CO2 的还原。这项研究为构建高性能 p-n 异质结光催化剂提供了一种很有前景的材料设计方法。
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引用次数: 0
Promoting effect of interfacial hole accumulation on photoelectrochemical water oxidation in BiVO4 and Mo-doped BiVO4 界面空穴积累对 BiVO4 和掺杂 Mo 的 BiVO4 中光电化学水氧化的促进作用
Pub Date : 2024-09-19 DOI: 10.1016/j.apmate.2024.100234
Xiaofeng Wu , Freddy E. Oropeza , Shixin Chang , Marcus Einert , Qingyang Wu , Clément Maheu , Julia Gallenberger , Chuanmu Tian , Kangle Lv , Jan P. Hofmann
Hole transfer at the semiconductor-electrolyte interface is a key elementary process in (photo)electrochemical (PEC) water oxidation. However, up to now, a detailed understanding of the hole transfer and the influence of surface hole density on PEC water oxidation kinetics is lacking. In this work, we propose a model for the first time in which the surface accumulated hole density in BiVO4 and Mo-doped BiVO4 samples during water oxidation can be acquired via employing illumination-dependent Mott-Schottky measurements. Based on this model, some results are demonstrated as below: (1) Although the surface hole density increases when increasing light intensity and applied potential, the hole transfer rate remains linearly proportional to surface hole density on a log-log scale. (2) Both water oxidation on BiVO4 and Mo-doped BiVO4 follow first-order reaction kinetics at low surface hole densities, which is in good agreement with literature. (3) We find that water oxidation active sites in both BiVO4 and Mo-doped BiVO4 are very likely to be Bi5+, which are produced by photoexcited or/and electro-induced surface holes, rather than VOx species or Mo6+ due to their insufficient redox potential for water oxidation. (4) Introduction of Mo doping brings about higher OER activity of BiVO4, as it suppresses the recombination rate of surface holes and increases formation of Bi5+. This surface hole model offers a general approach for the quantification of surface hole density in the field of semiconductor photoelectrocatalysis.
半导体-电解质界面上的空穴传输是(光)电化学(PEC)水氧化过程中的一个关键基本过程。然而,迄今为止,人们还缺乏对空穴传输以及表面空穴密度对 PEC 水氧化动力学影响的详细了解。在这项工作中,我们首次提出了一个模型,通过利用与光照相关的 Mott-Schottky 测量方法,可以获得水氧化过程中 BiVO4 和掺钼 BiVO4 样品的表面累积空穴密度。根据这一模型,得出了以下结果:(1) 虽然表面空穴密度随光照强度和外加电位的增加而增加,但空穴传输率仍与表面空穴密度成对数线性关系。(2) 水在 BiVO4 和掺 Mo 的 BiVO4 上的氧化反应在低表面空穴密度时都遵循一阶反应动力学,这与文献报道十分吻合。(3) 我们发现,BiVO4 和掺杂 Mo 的 BiVO4 中的水氧化活性位点很可能是由光激发或/和电诱导表面空穴产生的 Bi5+,而不是 VOx 物种或 Mo6+,因为它们的氧化还原电位不足以进行水氧化。(4) Mo 的掺杂抑制了表面空穴的重组速度,增加了 Bi5+ 的形成,从而提高了 BiVO4 的 OER 活性。这种表面空穴模型为量化半导体光电催化领域的表面空穴密度提供了一种通用方法。
{"title":"Promoting effect of interfacial hole accumulation on photoelectrochemical water oxidation in BiVO4 and Mo-doped BiVO4","authors":"Xiaofeng Wu ,&nbsp;Freddy E. Oropeza ,&nbsp;Shixin Chang ,&nbsp;Marcus Einert ,&nbsp;Qingyang Wu ,&nbsp;Clément Maheu ,&nbsp;Julia Gallenberger ,&nbsp;Chuanmu Tian ,&nbsp;Kangle Lv ,&nbsp;Jan P. Hofmann","doi":"10.1016/j.apmate.2024.100234","DOIUrl":"10.1016/j.apmate.2024.100234","url":null,"abstract":"<div><div>Hole transfer at the semiconductor-electrolyte interface is a key elementary process in (photo)electrochemical (PEC) water oxidation. However, up to now, a detailed understanding of the hole transfer and the influence of surface hole density on PEC water oxidation kinetics is lacking. In this work, we propose a model for the first time in which the surface accumulated hole density in BiVO<sub>4</sub> and Mo-doped BiVO<sub>4</sub> samples during water oxidation can be acquired via employing illumination-dependent Mott-Schottky measurements. Based on this model, some results are demonstrated as below: (1) Although the surface hole density increases when increasing light intensity and applied potential, the hole transfer rate remains linearly proportional to surface hole density on a log-log scale. (2) Both water oxidation on BiVO<sub>4</sub> and Mo-doped BiVO<sub>4</sub> follow first-order reaction kinetics at low surface hole densities, which is in good agreement with literature. (3) We find that water oxidation active sites in both BiVO<sub>4</sub> and Mo-doped BiVO<sub>4</sub> are very likely to be Bi<sup>5+</sup>, which are produced by photoexcited or/and electro-induced surface holes, rather than VO<sub><em>x</em></sub> species or Mo<sup>6+</sup> due to their insufficient redox potential for water oxidation. (4) Introduction of Mo doping brings about higher OER activity of BiVO<sub>4</sub>, as it suppresses the recombination rate of surface holes and increases formation of Bi<sup>5+</sup>. This surface hole model offers a general approach for the quantification of surface hole density in the field of semiconductor photoelectrocatalysis.</div></div>","PeriodicalId":7283,"journal":{"name":"Advanced Powder Materials","volume":"3 6","pages":"Article 100234"},"PeriodicalIF":0.0,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142434169","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Emerging semiconductor ionic materials tailored by mixed ionic-electronic conductors for advanced fuel cells 为先进燃料电池量身定制离子电子混合导体的新兴半导体离子材料
Pub Date : 2024-09-10 DOI: 10.1016/j.apmate.2024.100231
Bushra Bibi , Atif Nazar , Bin Zhu , Fan Yang , Muhammad Yousaf , Rizwan Raza , M.A.K. Yousaf Shah , Jung-Sik Kim , Muhammad Afzal , Yongpeng Lei , Yifu Jing , Peter Lund , Sining Yun
Mixed ionic-electronic conductors (MIECs) play a crucial role in the landscape of energy conversion and storage technologies, with a pronounced focus on electrode materials’ application in solid oxide fuel cells (SOFCs) and proton-conducting ceramic fuel cells (PCFCs). In parallel, the emergence of semiconductor ionic materials (SIMs) has introduced a new paradigm in the field of functional materials, particularly for both electrode and electrolyte development for low-temperature, 300–550 ​°C, SOFCs, and PCFCs. This review article critically delves into the intricate mechanisms underpinning the synergistic relationship between MIECs and SIMs, with a particular emphasis on elucidating the fundamental working principles of semiconductor ionic membrane fuel cells (SIMFCs). By exploring critical facets such as ion-coupled electron transfer/transport, junction effect, energy bands alignment, and theoretical computations, it casts an illuminating spotlight on the transformative potential of MIECs, also involving triple charge conducting oxides (TCOs) in the context of SIMs and advanced fuel cells (FCs). The insights and findings articulated herein contribute substantially to the advancement of SIMs and SIMFCs by tailoring MIECs (TCOs) as promising avenues toward the emergence of high-performance SIMFCs. This scientific quest not only addresses the insistent challenges surrounding efficient charge transfer, ionic transport and power output but also unlocks the profound potential for the widespread commercialization of FC technology.
混合离子电子导体(MIECs)在能源转换和储存技术领域发挥着至关重要的作用,其重点是电极材料在固体氧化物燃料电池(SOFCs)和质子传导陶瓷燃料电池(PCFCs)中的应用。与此同时,半导体离子材料(SIMs)的出现为功能材料领域引入了新的范式,特别是用于低温(300-550 °C)SOFC 和 PCFC 的电极和电解质开发。这篇综述文章批判性地探讨了 MIEC 和 SIMs 之间协同作用的复杂机制,尤其侧重于阐明半导体离子膜燃料电池(SIMFC)的基本工作原理。通过探索离子耦合电子转移/传输、结点效应、能带排列和理论计算等关键方面,该研究揭示了 MIECs 的变革潜力,还涉及 SIMs 和先进燃料电池(FCs)背景下的三电荷导电氧化物(TCOs)。本文所阐述的见解和发现,通过将 MIEC(三电荷导电氧化物)量身定做为实现高性能 SIMFC 的可行途径,极大地推动了 SIMs 和 SIMFC 的发展。这一科学探索不仅解决了围绕高效电荷转移、离子传输和功率输出的持续挑战,还为 FC 技术的广泛商业化释放了巨大潜力。
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引用次数: 0
Advances in powder nano-photocatalysts as pollutant removal and as emerging contaminants in water: Analysis of pros and cons on health and environment 粉末纳米光催化剂在去除污染物和作为水中新污染物方面的进展:健康与环境利弊分析
Pub Date : 2024-09-10 DOI: 10.1016/j.apmate.2024.100233
Sahil Thakur , Abhijeet Ojha , Sushil Kumar Kansal , Navneet Kumar Gupta , Hendrik C. Swart , Junghyun Cho , Andrej Kuznetsov , Shuhui Sun , Jai Prakash
Photocatalysis is an advanced oxidation process where light exposure triggers a semiconducting nanomaterial (nano-photocatalyst) to generate electron-hole (e/h+) pairs and free radicals. This phenomenon is widely used for the photocatalysis-assisted removal of organic and other contaminants using wide range of nano-photocatalysts, offering an efficient approach to environmental remediation. However, the introduction of powdered nano-photocatalysts into water systems often leads to unintended secondary pollution in the form of residual nano-photocatalysts, ion leaching, free radicals, toxic by-products etc. Such practices potentially introduce emerging secondary contaminants into aquatic environments, posing risks to both aquatic life and human health. The resulting chemical by-products and intermediates can effectively induce chronic toxicity, neurological and developmental disorders, cardiovascular defects, and intestinal ailments in humans and aquatic species. Despite having a range of health and environmental consequences, this dark side of nano-photocatalysts has been comparatively less explored and discussed in the literature. In this review, the pros and cons of powder nano-photocatalysts are discussed in view of their advantages as well as disadvantages in wastewater treatment. The discussion encompasses their classification based on composition, dimensions, structure, and activity, as well as recent advancements in improving their photocatalytic efficiency. The article also explores the recent advances on their applications in photocatalytic removal of various water pollutants/contaminants of emerging concern (i.e., organic pollutants, micro/nano plastics, heavy ions, disinfections, etc.) Furthermore, an emphasis on the role of such nano-photocatalysts as emerging (secondary) contaminants in water system, along with a thorough discussion of latest studies related to the health and environmental issues, has been discussed. Additionally, it addresses critical issues in applying powder nano-photocatalysts for wastewater detoxification and explores potential solutions to these challenges followed by future prospects.
光催化是一种先进的氧化过程,在这一过程中,光线照射会触发半导体纳米材料(纳米光催化剂)产生电子-空穴(e-/h+)对和自由基。这种现象被广泛用于光催化辅助去除有机物和其他污染物,使用的纳米光催化剂种类繁多,为环境修复提供了一种有效的方法。然而,将粉末状纳米光催化剂引入水系统往往会导致纳米光催化剂残留、离子沥滤、自由基、有毒副产品等形式的意外二次污染。这种做法可能会将新出现的二次污染物引入水生环境,对水生生物和人类健康构成风险。由此产生的化学副产品和中间体可有效诱发人类和水生生物的慢性中毒、神经和发育障碍、心血管缺陷和肠道疾病。尽管纳米光催化剂具有一系列健康和环境后果,但文献中对其阴暗面的探讨和讨论相对较少。本综述从纳米粉末光催化剂在废水处理中的利弊两方面进行了讨论。讨论内容包括根据成分、尺寸、结构和活性对其进行的分类,以及在提高其光催化效率方面的最新进展。文章还探讨了纳米光催化剂在光催化去除各种水污染物/新出现的污染物(如有机污染物、微/纳米塑料、重离子、消毒剂等)方面的最新应用进展。此外,文章还重点讨论了此类纳米光催化剂作为水系统中新出现的(二次)污染物的作用,并深入探讨了与健康和环境问题相关的最新研究。此外,报告还讨论了将粉末纳米光催化剂用于废水解毒的关键问题,并探讨了应对这些挑战的潜在解决方案以及未来前景。
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引用次数: 0
Surface engineering of nickel-rich single-crystal layered oxide cathode enables high-capacity and long cycle-life sulfide all-solid-state batteries 富镍单晶层状氧化物阴极的表面工程技术实现了高容量、长循环寿命的硫化物全固态电池
Pub Date : 2024-08-21 DOI: 10.1016/j.apmate.2024.100228
Xuebao Li , Jiasen Wang , Cheng Han , Kun Zeng , Zhuangzhi Wu , Dezhi Wang

Sulfide all-solid-state lithium batteries (SASSLBs) with a single-crystal nickel-rich layered oxide cathode (LiNixCoyMn1-x-yO2, x ​≥ ​0.8) are highly desirable for advanced power batteries owing to their excellent energy density and safety. Nevertheless, the cathode material's cracking issue and its severe interfacial problem with sulfide solid electrolytes have hindered the further development. This study proposes to employ surface modification engineering to produce B-NCM cathode materials coated with boride nanostructure stabilizer in situ by utilizing NCM encapsulated with residual lithium. This approach enhances the electrochemical performance of SASSLBs by effectively inhibiting electrochemical-mechanical degradation of the NCM cathode material on cycling and reducing deleterious side reactions with the solid sulfide electrolyte. The B-NCM/LPSCl/Gr SASSLBs demonstrate impressive cycling stability, retaining 84.19 ​% of its capacity after 500 cycles at 0.2 ​C, which represents a 30.13 ​% increase vs. NCM/LPSCl/Gr. It also exhibits a specific capacity of 170.4 mAh/g during its first discharge at 0.1 ​C. This work demonstrates an effective surface engineering strategy for enhancing capacity and cycle life, providing valuable insights into solving interfacial problems in SASSLBs.

采用单晶富镍层状氧化物正极(LiNixCoyMn1-x-yO2,x ≥ 0.8)的硫化物全固态锂电池(SASSLBs)具有出色的能量密度和安全性,是先进动力电池的理想选择。然而,阴极材料的开裂问题及其与硫化物固体电解质的严重界面问题阻碍了其进一步发展。本研究提出采用表面改性工程技术,利用残留锂包裹的 NCM,在原位生产涂有硼化物纳米结构稳定剂的 B-NCM 正极材料。这种方法可有效抑制 NCM 阴极材料在循环过程中的电化学-机械降解,并减少与固体硫化物电解质的有害副反应,从而提高 SASSLB 的电化学性能。B-NCM/LPSCl/Gr SASSLBs 的循环稳定性令人印象深刻,在 0.2 C 下循环 500 次后,其容量保持率为 84.19%,与 NCM/LPSCl/Gr 相比提高了 30.13%。这项工作展示了一种提高容量和循环寿命的有效表面工程策略,为解决 SASSLB 的界面问题提供了宝贵的见解。
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引用次数: 0
New lead-free chemistry for in-situ monitoring of advanced nuclear power plant 用于先进核电站原位监测的新型无铅化学材料
Pub Date : 2024-08-17 DOI: 10.1016/j.apmate.2024.100229
Lexing Liang , Xiuling Wang , Cong Zhang , Kailei Lu , Guangfan Tan , Yanhao Dong , Yanli Shi , Jianqi Qi , Tiecheng Lu

Nuclear power is essential for sustainable energy infrastructure and economic development, necessitating materials for high-radiation environments that can facilitate visualization and observation. Conventional lead glass is inadequate for future requirements due to radiation-induced darkening, poor mechanical properties, and toxicity. Therefore, there is urgent to find new window materials that offer multi-ionization shielding (particularly against deep-penetrating gamma ray, γ, and neutron, n, radiations), desirable opto-mechanical properties, service stability against darkening, and non-toxicity. In this study, we report a family of transparent rare-earth pyrochlore ceramics LaxGd2−xZr2O7, offering unique chemo-physical properties that are ideal for robust radiation shielding windows. Remarkably, we demonstrated the capability of maintaining high transparency under heavy-dose exposure to 1000 ​kGy 60Co γ radiation. We observed the service stability against radiation darkening can be greatly enhanced with La-rich compositions, while Gd-rich compositions undergo shallow darkening that can be reversibly recovered under visible light. This behavior is attributed to mitigated oxygen migration from 48f to 8a in La-rich compositions, which have high pyrochlore phase stability and well-ordered atomic structures, and reversible oxygen migration between 48f and 8a in Gd-rich compositions, which remain active at room temperature. Our proposal and demonstration unlock ample opportunities in designing functional transparent ceramics as window materials for demanding applications in high-radiation environments.

核电对可持续能源基础设施和经济发展至关重要,因此需要可用于高辐射环境的材料,以方便可视化和观察。传统的铅玻璃由于辐射引起的暗化、机械性能差和毒性等问题,已无法满足未来的要求。因此,急需找到能提供多电离屏蔽(特别是针对深穿透伽马射线(γ)和中子辐射(n))、理想的光学机械性能、防变黑的服役稳定性和无毒性的新型窗户材料。在这项研究中,我们报告了一系列透明的稀土热长石陶瓷 LaxGd2-xZr2O7,它们具有独特的化学物理特性,是坚固耐用的辐射屏蔽窗的理想材料。值得注意的是,我们展示了在 1000 kGy 60Co γ 重剂量辐射下保持高透明度的能力。我们观察到,富含 La 的成分可大大提高抗辐射变暗的稳定性,而富含 Gd 的成分则会出现浅度变暗,但在可见光下可逆恢复。这种行为归因于富含 La 的成分中从 48f 到 8a 的氧迁移得到了缓解,La 具有较高的热释电晶体相稳定性和有序的原子结构,而富含 Gd 的成分中从 48f 到 8a 的氧迁移是可逆的,Gd 在室温下保持活跃。我们的建议和演示为设计功能性透明陶瓷提供了大量机会,可将其作为窗口材料,用于高辐射环境中的苛刻应用。
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Advanced Powder Materials
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