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Performance evaluation of a newly developed transition metal-doped HZSM-5 zeolite catalyst for single-step conversion of C1–C3 alcohols to fuel-range hydrocarbons† 新开发的掺杂过渡金属的 HZSM-5 沸石催化剂在将 C1-C3 醇单步转化为燃料级碳氢化合物中的性能评估
Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-05-29 DOI: 10.1039/D3YA00460K
Ifeanyi Michael Smarte Anekwe, Bilainu Oboirien and Yusuf Makarfi Isa

This study investigated the performance of metal-doped HZSM-5 catalysts in the conversion of low alcohols to hydrocarbons (LATH). Catalysts, including unmodified HZSM-5 and metal-modified (Ni, Fe, and Co) HZSM-5, were evaluated at 350 and 400 °C with space velocities of 7 and 12 h−1 for LATH conversion. Characterisation techniques such as XRD, FTIR, SEM-EDS, PSD, N2 adsorption, and TGA-DTA were employed. The characterisation results showed the successful metal incorporation in the HZSM-5 support catalyst. The overall evaluation of catalyst performance for LATH conversion revealed that the metal-doped catalysts showed a clear preference for liquid hydrocarbons with >99% average low alcohol conversion compared to the unmodified catalysts. In particular, Co/HZSM-5 and Fe/HZSM-5 showed a considerable preference for C5–C8 (62.81% and 54.95%), while Ni/HZSM-5 improved the synthesis of C9–C12 (11.40%), C12+ (20.91%) and BTX (7.01%). The study on coke deposition indicated that Ni/HZSM-5 exhibited stability with minimal coke formation, while Co/HZSM-5 experienced higher coke deposition and deactivation tendencies in MTH and ETH conversions, respectively. Co/HZSM-5 exhibited the lowest weight loss, whereas Fe/HZSM-5 showed lower stability in PTH conversion. Notably, Ni/HZSM-5 demonstrated remarkable stability and performance in LATH conversion. These findings contribute to the advancement of catalysis and the transition towards a sustainable energy future.

本研究调查了掺杂金属的 HZSM-5 催化剂在低醇转化为碳氢化合物(LATH)中的性能。对催化剂(包括未改性 HZSM-5 和金属改性(镍、铁和钴)HZSM-5)在 350 和 400 °C、7 和 12 h-1 的空间速度下进行了 LATH 转化评估。采用了 XRD、FTIR、SEM-EDS、PSD、N2 吸附和 TGA-DTA 等表征技术。表征结果表明,金属成功地掺入了 HZSM-5 载体催化剂中。对 LATH 转化催化剂性能的整体评估表明,与未改性催化剂相比,掺杂金属的催化剂明显更偏向于液态烃,平均低醇转化率为 99%。其中,Co/HZSM-5 和 Fe/HZSM-5 对 C5-C8 (62.81% 和 54.95%)有明显的偏好,而 Ni/HZSM-5 则改善了 C9-C12 (11.40%)、C12+ (20.91%)和 BTX (7.01%)的合成。对焦炭沉积的研究表明,Ni/HZSM-5 具有稳定性,焦炭形成极少,而 Co/HZSM-5 在 MTH 和 ETH 转化中分别具有较高的焦炭沉积和失活倾向。Co/HZSM-5 的失重率最低,而 Fe/HZSM-5 在 PTH 转化中的稳定性较低。值得注意的是,Ni/HZSM-5 在 LATH 转化中表现出卓越的稳定性和性能。这些发现有助于催化技术的进步和向可持续能源未来的过渡。
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引用次数: 0
Performance and failure mechanisms of alkaline zinc anodes with addition of calcium zincate (Ca[Zn(OH)3]2·2H2O) under industrially relevant conditions† 添加锌酸钙(Ca[Zn(OH)3]2-2H2O)的碱性锌阳极在工业相关条件下的性能和失效机理
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-05-28 DOI: 10.1039/D4YA00093E
Patrick K. Yang, Damon E. Turney, Michael Nyce, Bryan R. Wygant, Timothy N. Lambert, Stephen O'Brien, Gautam G. Yadav, Meir Weiner, Shinju Yang, Brendan E. Hawkins and Sanjoy Banerjee

Additions of calcium zincate (CaZn2(OH)6·2H2O, CaZn) to zinc (Zn) anodes in alkaline batteries have been investigated and were found to remarkably increase cycle life at high 50% Zn utilization of the anode's theoretical capacity, thereby significantly reducing anode costs. A spectrum of anode formulations with increasing CaZn (0%, 30%, 70%, 100%) in mixtures with metallic Zn is investigated along with minor additions of Bi2O3, acetylene carbon black, and CTAB. The total molar zinc content is normalized; thus, electrode capacity is kept comparable, resulting in electrodes relevant to real world use cases. We report details of the cell design, electrolyte composition, electrode design, and cycle testing procedure, all of which are kept close to industrially relevant values. A pure CaZn anode with acetylene carbon was shown to achieve 1062 cycles at 20% Zn utilization in ZnO saturated 20 wt% KOH whereas traditional Zn anodes only utilize 10% for similar cycle life. At high 50% Zn utilization, CaZn anodes achieved ∼280 cycles while Zn anodes achieved ∼50 cycles, resulting in a five-fold improvement in cycle life resulting in approximately ∼25% reduction in cost per cycle. Scanning electron microscopy analysis of cycled electrodes shows that adding CaZn reduces electrode failure by slowing down formation of a passivating zinc oxide layer at the surface of the electrode as well as decreases shape change. This appears to occur because zinc and calcium remain intimately mixed forming CaZn, which reduces dissolution and reprecipitation, but slowly will segregate as inactive materials are pushed to the surface where conductivity is lower.

研究发现,在碱性电池的锌(Zn)阳极中添加锌酸钙(CaZn2(OH)6∙2H2O)可在较高的阳极理论容量利用率下显著延长循环寿命,从而大幅降低阳极成本。研究了在与金属锌的混合物中增加 CaZn(0%、30%、70%、100%)以及少量添加 Bi2O3、乙炔碳和 CTAB 的阳极配方。总摩尔锌含量已归一化;因此,电极容量保持可比,从而使电极与现实世界中的应用案例相关。我们报告了电池设计、电解质成分、电极设计和循环测试程序的细节,所有这些都与工业相关值保持一致。结果表明,在氧化锌饱和的 20 wt.% KOH 中,纯 CaZn 阳极与乙炔碳在 20% 的锌利用率下可实现 1062 个循环,而传统的锌阳极在类似的循环寿命下仅能利用 10% 的锌。在锌利用率高达 50%的情况下,钙锌阳极可实现约 280 个循环,而锌阳极只能实现约 50 个循环,循环寿命提高了五倍,每个循环的成本降低了四倍。对循环电极的扫描电子显微镜分析表明,添加 CaZn 可减缓电极表面钝化氧化锌层的形成,从而减少电极故障,并降低形状变化。出现这种情况似乎是因为锌和钙保持紧密混合形成了 CaZn,从而减少了溶解和再沉淀,但随着非活性材料被推向导电率较低的表面,它们会慢慢分离。
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引用次数: 0
Nickel polyelectrolytes as hole transporting materials for organic and perovskite solar cell applications† 将镍多电解质作为有机和包光体太阳能电池应用的空穴传输材料
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-05-27 DOI: 10.1039/D4YA00081A
Jin Hee Lee, Kausar Ali Khawaja, Faiza Shoukat, Yeasin Khan, Do Hui Kim, Shinuk Cho, Bright Walker and Jung Hwa Seo

Engineering interfacial materials for use between the active layer and the electrodes in organic and perovskite solar cells is one of the most effective ways to increase device efficiency. Despite decades of development, new materials continue to emerge offering improved performance and streamlined fabrication of devices. Here, a hole transport layer (HTL) for organic and perovskite solar cells combining poly(styrene sulfonate) (PSS) and nickel (Ni2+) is presented. P-type carriers and p-doping at the anode are stabilized by the PSS backbone's negatively charged state. The impact of ionic moieties on the electronic band structure and characteristics of organic and perovskite solar cells must be understood. The combination of Nickel(II): poly(styrene sulfonate) (Ni:PSS) and poly(3,4-ethylenedioxythiophene): poly(styrene sulfonate) (PEDOT:PSS) can improve efficiency to 15.67% (perovskite solar cell) and 16.90% (organic solar cell) over traditional Ni:PSS and PEDOT:PSS. Ultraviolet photoelectron spectroscopic observations at HTL/donor interfaces indicate energy level alignment, which is the cause of various changes in device performance. Low ionization potential (IP) and hole injection barrier (ϕh) are essential at the HTL/donor interface for effective charge extraction in organic and perovskite solar cells.

在有机太阳能电池和过氧化物太阳能电池的活性层和电极之间使用界面材料是提高设备效率的最有效方法之一。尽管经过几十年的发展,新材料仍在不断涌现,从而提高了性能并简化了设备的制造,但人们对离子分子对有机和包光体太阳能电池的电子带结构和特性的影响仍不完全了解。本文介绍了结合聚苯乙烯磺酸盐(PSS)和镍(Ni2+)的有机和包光体太阳能电池空穴传输层(HTL)。阳极的 P 型载流子和 p 型掺杂稳定了 PSS 骨架的负电荷状态。镍 (II):聚苯乙烯磺酸盐(Ni:PSS)和聚(3,4-亚乙二氧基噻吩):聚苯乙烯磺酸盐(PEDOT:PSS)的组合可将效率提高到 15.67%(过氧化物太阳能电池)和 16.90%(有机太阳能电池);与单组分的 Ni:PSS 和 PEDOT:PSS HTL 相比有显著提高。在 HTL/供体界面上进行的紫外光电子能谱观测揭示了能级排列,这导致了器件性能的各种变化。低电离势(IP)和空穴注入势垒(jh)对 HTL/载体界面在有机和过氧化物太阳能电池中有效提取电荷至关重要。
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引用次数: 0
Optimizing direct air capture under varying weather conditions† 在不同天气条件下优化直接空气捕获
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-05-27 DOI: 10.1039/D4YA00200H
H. M. Schellevis, J. D. de la Combé and D. W. F. Brilman

CO2 from adsorption with supported-amine sorbents using steam-assisted temperature-vacuum swing adsorption is a technology to capture CO2 from the atmosphere (direct air capture). This process has many operational parameters and, on top of that, is heavily influenced by the ambient temperature and relative humidity. Identifying the minimum cost of direct air capture becomes a multi-dimensional problem in which climate conditions has to be incorporated as well. This study aims to evaluate the cost of direct air capture for year-round operation and to relate this to climate conditions. An optimization framework was developed with the ambient conditions as input parameters. This framework is able to find the minimum cost of direct air capture for a given fixed bed DAC facility and provides the corresponding operational parameters. These results were coupled to year-round weather data to find the total costs for continuous operation. We showed that the cost of CO2 capture from air correlates well with the average annual temperature, with a high average temperature being more beneficial. Furthermore, climates with strong variation in weather conditions over the seasons require dynamic process control in order to operate at minimum cost of DAC. Overall, the presented optimization framework is an excellent tool to identify suitable locations for direct air capture and provide the operational parameters to minimize its cost.

利用蒸汽辅助温度-真空变温吸附技术,使用支撑胺吸附剂吸附大气中的二氧化碳是一种从大气中捕获二氧化碳的技术(直接空气捕获)。该工艺有许多操作参数,而且受环境温度和相对湿度的影响很大。确定直接空气捕集的最低成本是一个多维度的问题,其中还必须考虑气候条件。本研究旨在评估全年运行的直接空气捕获成本,并将其与气候条件联系起来。以环境条件为输入参数,开发了一个优化框架。该框架能够为给定的固定床 DAC 设施找到直接空气捕集的最低成本,并提供相应的运行参数。将这些结果与全年天气数据相结合,可得出连续运行的总成本。我们的研究表明,从空气中捕获二氧化碳的成本与年平均气温密切相关,平均气温越高越有利。此外,在气候条件四季变化较大的情况下,需要进行动态过程控制,以便以最低的 DAC 成本运行。总之,所提出的优化框架是一个极好的工具,可用于确定直接空气捕集的合适地点,并提供运行参数,使其成本最小化。
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引用次数: 0
Strategic Ni-doping improved electrocatalytic H2 production by Bi3O4Br in alkaline water† 策略性掺杂镍改善了 Bi3O4Br 在碱性水中的电催化 H2 产率
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-05-24 DOI: 10.1039/D4YA00228H
Manodip Pal, Rathindranath Biswas, Sanmitra Barman and Arnab Dutta

Establishing a cost-effective and efficient electrocatalytic pathway for the hydrogen evolution reaction (HER) is the key to our quest for a carbon-neutral energy landscape. We report a simple and straightforward approach to synthesize an efficient, stable, and low-cost noble metal-free Bi3O4Br electrocatalyst. Tactical doping of Ni ions into Bi3O4Br effectively enhanced the conductivity, accelerated the charge transfer process, and provided more catalytic active sites to significantly boost the alkaline electrochemical HER performance of Bi3O4Br. This Ni-doped Bi3O4Br exhibited a lower overpotential of 662 mV compared to that of Bi3O4Br (736 mV) at a higher current density (50 mA cm−2). Additionally, the HER kinetics were also enhanced in terms of Tafel slope for this doped material (159 mV dec−1) compared to the pristine Bi3O4Br (245 mV dec−1), which coincides with a significant improvement in the mass activity (52 A g−1 to 98 A g−1). Notably, the overpotential of Ni-doped Bi3O4Br was further reduced to 614 mV at the same current density of 50 mA cm−2 during photoelectrochemical HER performance testing, and the faradaic efficiency was improved from 79% to 87%. Finally, an enhanced durability of the material was observed for Bi3O4Br following the Ni-doping. Hence, this strategy highlights the importance of unravelling upgraded catalytic behaviour for abundant materials with rational doping.

为氢进化反应(HER)建立一种经济高效的电催化途径是我们实现碳中和能源格局的关键。我们报告了一种简单直接的方法来合成高效、稳定和低成本的无贵金属 Bi3O4Br 电催化剂。在 Bi3O4Br 中战术性地掺入镍离子可有效提高电导率,加速电荷转移过程,并提供更多的催化活性位点,从而显著提高 Bi3O4Br 的碱性电化学 HER 性能。 这种掺镍的 Bi3O4Br 在更高的电流密度(100 mA/cm2)下工作时,能量效率提高了 17%。此外,与原始 Bi3O4Br 相比,这种掺杂材料的 HER 动力学在塔菲尔斜率方面也提高了 35%,这与质量活性的显著提高(从 52 A/g 提高到 98 A/g)相吻合。值得注意的是,掺杂镍的 Bi3O4Br 在光电化学 HER 性能中的过电位进一步降低了 23%,法拉第效率提高了 10%。最后,掺杂镍后,Bi3O4Br 材料的耐久性得到了提高。因此,这一策略强调了通过合理掺杂来揭示丰富材料的升级催化行为的重要性。
{"title":"Strategic Ni-doping improved electrocatalytic H2 production by Bi3O4Br in alkaline water†","authors":"Manodip Pal, Rathindranath Biswas, Sanmitra Barman and Arnab Dutta","doi":"10.1039/D4YA00228H","DOIUrl":"10.1039/D4YA00228H","url":null,"abstract":"<p >Establishing a cost-effective and efficient electrocatalytic pathway for the hydrogen evolution reaction (HER) is the key to our quest for a carbon-neutral energy landscape. We report a simple and straightforward approach to synthesize an efficient, stable, and low-cost noble metal-free Bi<small><sub>3</sub></small>O<small><sub>4</sub></small>Br electrocatalyst. Tactical doping of Ni ions into Bi<small><sub>3</sub></small>O<small><sub>4</sub></small>Br effectively enhanced the conductivity, accelerated the charge transfer process, and provided more catalytic active sites to significantly boost the alkaline electrochemical HER performance of Bi<small><sub>3</sub></small>O<small><sub>4</sub></small>Br. This Ni-doped Bi<small><sub>3</sub></small>O<small><sub>4</sub></small>Br exhibited a lower overpotential of 662 mV compared to that of Bi<small><sub>3</sub></small>O<small><sub>4</sub></small>Br (736 mV) at a higher current density (50 mA cm<small><sup>−2</sup></small>). Additionally, the HER kinetics were also enhanced in terms of Tafel slope for this doped material (159 mV dec<small><sup>−1</sup></small>) compared to the pristine Bi<small><sub>3</sub></small>O<small><sub>4</sub></small>Br (245 mV dec<small><sup>−1</sup></small>), which coincides with a significant improvement in the mass activity (52 A g<small><sup>−1</sup></small> to 98 A g<small><sup>−1</sup></small>). Notably, the overpotential of Ni-doped Bi<small><sub>3</sub></small>O<small><sub>4</sub></small>Br was further reduced to 614 mV at the same current density of 50 mA cm<small><sup>−2</sup></small> during photoelectrochemical HER performance testing, and the faradaic efficiency was improved from 79% to 87%. Finally, an enhanced durability of the material was observed for Bi<small><sub>3</sub></small>O<small><sub>4</sub></small>Br following the Ni-doping. Hence, this strategy highlights the importance of unravelling upgraded catalytic behaviour for abundant materials with rational doping.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 7","pages":" 1562-1570"},"PeriodicalIF":3.2,"publicationDate":"2024-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ya/d4ya00228h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141147707","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
Dynamic synergy of tin in the electron-transfer layer and absorber layer for advancing perovskite solar cells: a comprehensive review 电子传输层和吸收层中锡的动态协同作用促进了过氧化物太阳能电池的发展:全面综述
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-05-23 DOI: 10.1039/D4YA00204K
Azaharuddin Saleem Shaikh, Subhash Chand Yadav, Abhishek Srivastava, Archana R. Kanwade, Manish Kumar Tiwari, Shraddha Manohar Rajore, Jena Akash Kumar Satrughna, Mahesh Dhonde and Parasharam M. Shirage

The landscape of metal halide-perovskite solar cells (MH-PSCs) has witnessed significant progress in terms of efficiency over the past decade. Nevertheless, concerns over the toxicity of lead (Pb)-based perovskite structures have restrained their full market potential. In response, the exploration of Sn perovskites has emerged as a promising alternative, fueled by their narrow band gaps, superior carrier mobilities, low-temperature production, economic viability, and reduced hysteresis. These Sn perovskites exhibit competitive PCE while addressing the toxicity issues of Pb-based PSCs. This comprehensive review delves into the pivotal role of Sn in advancing PSCs, offering a consolidated understanding of its multifaceted applications. The report extensively examines the incorporation of Sn-based electron-transfer layers (ETLs) and absorber layers within PSCs, encompassing various dimensions, such as synthesis techniques, optoelectrical features, the future of Pb-free solar cells, integration into double PSCs, and the impact of doping strategies. Finally, this review proposes the future perspectives and investigations needed to make Sn-based PSCs a viable alternative to Pb-based MH-PSCs.

过去十年间,金属卤化物-过氧化物太阳能电池(MH-PSCs)在效率方面取得了重大进展。然而,人们对铅(Pb)基过氧化物结构毒性的担忧限制了其市场潜力的充分发挥。作为回应,对锡包晶石的探索已成为一种很有前景的替代方案,因为它们具有带隙窄、载流子迁移率高、低温生产、经济可行以及磁滞减少等优点。这些锡类过氧化物在解决毒性问题的同时,还表现出具有竞争力的 PCE。本综述深入探讨了锡在促进 PSCs 发展中的关键作用,对其多方面的应用提供了全面的了解。报告广泛探讨了在 PSCs 中加入锡基电子转移层 (ETL) 和吸收层的问题,涉及合成技术、光电特性、无铅太阳能电池的未来、双 PSCs 的集成以及掺杂策略的影响等多个方面。此外,本综述最后还提出了使无铅太阳能电池成为基于铅的 MH-PSCs 的可行替代品所需的未来展望和研究。
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引用次数: 0
Evaluation of zinc sulfide heterostructures as catalysts for the transformation of CO2 into valuable chemicals and clean energy generation 评估硫化锌异质结构作为将二氧化碳转化为有价值化学品和清洁能源的催化剂的效果
Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-05-23 DOI: 10.1039/D4YA00202D
Onome Ejeromedoghene, Khadijat Olabisi Abdulwahab, Inemesit Asukwo Udofia, Moses Kumi and Ayorinde Olufunke Nejo

There are significant concerns about global warming and the energy crisis due to the rise in atmospheric carbon dioxide (CO2) concentration and the depletion of fossil fuels. Converting CO2 into organic molecules using the abundant solar energy would be a quick fix that would address both issues. Excess CO2 is a major contributor to the greenhouse effect, which leads to global warming, extreme weather patterns, and a host of other environmental challenges. To tackle these problems, scientists are exploring novel approaches to adsorb CO2, transform it into useful products, and then release it back into the atmosphere. Semiconductor materials play a crucial role in CO2 reduction. Among these materials, zinc sulfide (ZnS) and doped ZnS have gained significant attention for the potential catalytic transformation of CO2 into useful compounds. The semiconductor properties of ZnS and its derivatives make them particularly well-suited for this purpose. The present review provides a summary of the recent progress in the development of strategies for fabricating ZnS-based heterostructures with functional properties for CO2 reduction. The mechanism of CO2 conversion was also addressed with new insights into computational modelling. Lastly, future outlook on the development of catalytic ZnS-based materials for CO2 reduction is provided.

由于大气中二氧化碳(CO2)浓度的上升和化石燃料的枯竭,全球变暖和能源危机备受关注。利用丰富的太阳能将二氧化碳转化为有机分子将是解决这两个问题的快速方法。过量的二氧化碳是导致全球变暖、极端天气模式和其他一系列环境挑战的温室效应的主要因素。为了解决这些问题,科学家们正在探索吸附二氧化碳的新方法,将其转化为有用的产品,然后再释放回大气中。半导体材料在二氧化碳还原过程中发挥着至关重要的作用。在这些材料中,硫化锌(ZnS)和掺杂 ZnS 因可能催化二氧化碳转化为有用化合物而备受关注。ZnS 及其衍生物的半导体特性使其特别适合于这一目的。本综述概述了在开发具有二氧化碳还原功能特性的 ZnS 基异质结构方面的最新进展。本综述还探讨了二氧化碳的转化机制,并对计算建模提出了新的见解。最后,还对用于还原二氧化碳的 ZnS 基催化材料的未来发展进行了展望。
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引用次数: 0
Stabilization of the surface and lattice structure for LiNi0.83Co0.12Mn0.05O2via B2O3 atomic layer deposition and post-annealing† 通过 B2O3 原子层沉积和后退火稳定 LiNi0.83Co0.12Mn0.05O2 的表面和晶格结构
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-05-22 DOI: 10.1039/D4YA00206G
Jiawei Li, Junren Xiang, Ge Yi, Zhijia Hu, Xiao Liu and Rong Chen

The Ni-rich LiNixCoyMn1−xyO2 cathode (x ≥ 0.6) shows weak rate capability due to its deleterious surface lithium impurities and lattice defects. Herein, uniform ultrathin B2O3 coatings built by atomic layer deposition (ALD) are utilized to construct a B3+ doped single-crystal LiNi0.83Co0.12Mn0.05O2 (SC83) via post-annealing. LiOH is consumed due to reacting with B2O3 during the B2O3 ALD process, and then B2O3 is transformed into B3+ doping accompanied by the reduction of Li2CO3 during the post-annealing. Surface and bulk characterization results show that B3+ tends to diffuse into the bulk of the SC83 during the post-annealing, which expands the a and c axes and reduces the Li+/Ni2+ mixing of the SC83. When the B3+ content exceeds 0.54 wt%, B3+ segregation occurs on the surface of the SC83, which decreases the electronic conductivity of the SC83. B3+ doping at the content of 0.54 wt% gives the highest capacity of 177.6 mA h g−1 at 1C rate. The B2O3 ALD coupled with post-annealing builds a highly electronic and Li+ conductive surface and bulk for the SC83, which is the key to the improvement of the rate capability.

富含镍的 LiNixCoyMn1-x-yO2 正极(x ≥ 0.6)因其有害的表面锂杂质和晶格缺陷而显示出较低的速率能力。在这里,利用原子层沉积(ALD)技术形成的均匀超薄 B2O3 涂层,通过后退火构建了掺杂 B3+ 的单晶 LiNi0.83Co0.12Mn0.05O2 (SC83)。在 B2O3 ALD 过程中,LiOH 与 B2O3 反应而被还原,然后在后退火过程中,B2O3 与 Li2CO3 的还原一起转化为 B3+掺杂。表面和块体表征显示,在后退火过程中,B3+趋向于扩散到 SC83 的块体中,从而扩大了 a 轴和 c 轴,降低了 SC83 的 Li+/Ni2+ 混合程度。当 B3+ 含量超过 0.54 wt.‰时,B3+ 会在 SC83 表面发生偏析,从而降低 SC83 的电子电导率。B3+ 掺杂含量为 0.54 重量.‰时,在 1C 速率下的容量最高,为 177.6 mAh/g。B2O3 ALD 与后退火相结合,为 SC83 构建了一个高电子和 Li+ 导电的表面和块体,这是提高速率能力的关键。
{"title":"Stabilization of the surface and lattice structure for LiNi0.83Co0.12Mn0.05O2via B2O3 atomic layer deposition and post-annealing†","authors":"Jiawei Li, Junren Xiang, Ge Yi, Zhijia Hu, Xiao Liu and Rong Chen","doi":"10.1039/D4YA00206G","DOIUrl":"10.1039/D4YA00206G","url":null,"abstract":"<p >The Ni-rich LiNi<small><sub><em>x</em></sub></small>Co<small><sub><em>y</em></sub></small>Mn<small><sub>1−<em>x</em>−<em>y</em></sub></small>O<small><sub>2</sub></small> cathode (<em>x</em> ≥ 0.6) shows weak rate capability due to its deleterious surface lithium impurities and lattice defects. Herein, uniform ultrathin B<small><sub>2</sub></small>O<small><sub>3</sub></small> coatings built by atomic layer deposition (ALD) are utilized to construct a B<small><sup>3+</sup></small> doped single-crystal LiNi<small><sub>0.83</sub></small>Co<small><sub>0.12</sub></small>Mn<small><sub>0.05</sub></small>O<small><sub>2</sub></small> (SC83) <em>via</em> post-annealing. LiOH is consumed due to reacting with B<small><sub>2</sub></small>O<small><sub>3</sub></small> during the B<small><sub>2</sub></small>O<small><sub>3</sub></small> ALD process, and then B<small><sub>2</sub></small>O<small><sub>3</sub></small> is transformed into B<small><sup>3+</sup></small> doping accompanied by the reduction of Li<small><sub>2</sub></small>CO<small><sub>3</sub></small> during the post-annealing. Surface and bulk characterization results show that B<small><sup>3+</sup></small> tends to diffuse into the bulk of the SC83 during the post-annealing, which expands the <em>a</em> and <em>c</em> axes and reduces the Li<small><sup>+</sup></small>/Ni<small><sup>2+</sup></small> mixing of the SC83. When the B<small><sup>3+</sup></small> content exceeds 0.54 wt%, B<small><sup>3+</sup></small> segregation occurs on the surface of the SC83, which decreases the electronic conductivity of the SC83. B<small><sup>3+</sup></small> doping at the content of 0.54 wt% gives the highest capacity of 177.6 mA h g<small><sup>−1</sup></small> at 1C rate. The B<small><sub>2</sub></small>O<small><sub>3</sub></small> ALD coupled with post-annealing builds a highly electronic and Li<small><sup>+</sup></small> conductive surface and bulk for the SC83, which is the key to the improvement of the rate capability.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 7","pages":" 1688-1696"},"PeriodicalIF":3.2,"publicationDate":"2024-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ya/d4ya00206g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141147705","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
Construction of a supramolecular light-harvesting system based on pillar[5]arene-mediated nanoparticles in water† 在水中构建基于支柱[5]炔介导纳米粒子的超分子光收集系统
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-05-22 DOI: 10.1039/D4YA00252K
Xiuxiu Li, Qiaona Zhang, Xiaoman Dang, Fengyao Cui, Zheng-Yi Li, Xiao-Qiang Sun and Tangxin Xiao

Light harvesting and energy transfer are ubiquitous processes in natural photosynthesis, significantly advancing the widespread utilization of solar energy. In this study, we engineered a supramolecular light-harvesting system utilizing a pyridinium salt-modified cyanostilbene guest (CPy) and a water-soluble pillar[5]arene host (WP5). Through host–guest complexation between WP5 and CPy, the resultant supra-amphiphile further self-assembled into emissive nanoparticles within aqueous environments. Incorporating the commercially available dye DBT into these nanoparticles yielded an efficient artificial light-harvesting system with a high donor/acceptor ratio (>200). Additionally, this system demonstrated tunable fluorescence emission in the solid state and exhibited potential applications as a color-tunable fluorescent ink for information encryption. Our findings not only delineate a promising approach for fabricating efficient light-harvesting systems via a straightforward supramolecular strategy but also underscore the significant potential of tunable photoluminescent nanomaterials.

光收集和能量传递是自然光合作用中无处不在的过程,极大地推动了太阳能的广泛利用。在这项研究中,我们利用吡啶鎓盐修饰的氰苯乙烯客体(CPy)和水溶性支柱[5]炔宿主(WP5)设计了一种超分子光收集系统。通过 WP5 和 CPy 之间的主客复合物,产生的超双亲化合物在水环境中进一步自组装成发射性纳米粒子。在这些纳米颗粒中加入市售染料 DBT,可产生一种高效的人工光收集系统,其供体/受体比高达(>200)。此外,该系统还展示了固态下的可调荧光发射,具有作为信息加密用颜色可调荧光墨水的潜在应用价值。我们的研究结果不仅为通过直接的超分子策略制造高效光收集系统提供了一种可行的方法,而且凸显了可调谐光致发光纳米材料的巨大潜力。
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引用次数: 0
Design and performance evaluation of all-inorganic AgTaS3 perovskite solar cells 全无机 AgTaS3 Perovskite 太阳能电池的设计与性能评估
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-05-22 DOI: 10.1039/D4YA00210E
Tanvir Ahmed, Md. Choyon Islam, Md. Alamin Hossain Pappu, Md. Islahur Rahman Ebon, Sheikh Noman Shiddique, Mainul Hossain and Jaker Hossain

Narrow bandgap AgTaS3 perovskite can offer highly efficient thin film solar cells (SCs) and become Si counterparts that are leading in the market. Herein, we study the response of a n-CdS/p-AgTaS3/p+-Al0.8Ga0.2Sb device according to the variation of thickness, doping concentration, and defect densities in each layer using a solar cell capacitance simulator (SCAPS-1D). The optimized cell shows a VOC of 0.78 V, PCE of 27.89% accompanied by a JSC of 46.37 mA cm−2, and a fill factor of 77.06%, paving the way for novel double heterojunction perovskite photovoltaic (PV) cells with remarkable performance.

窄带隙 AgTaS3 包晶可以提供高效薄膜太阳能电池(SC),并成为市场上领先的硅太阳能电池。在此,我们利用太阳能电池电容模拟器(SCAPS-1D)研究了 n-CdS/p-AgTaS3/p+-Al0.8Ga0.2Sb 器件在厚度、掺杂浓度和各层缺陷密度变化时的响应。优化后的电池显示出 0.78 V 的 VOC、27.89% 的 PCE 和 46.37 mA/cm2 的 JSC,以及 77.06% 的填充因子,为性能卓越的新型双异质结包晶光伏(PV)电池铺平了道路。
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Energy advances
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