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Amorphous carbon intercalated MoS2 nanosheets embedded on reduced graphene oxide for excellent high-rate and ultralong cycling sodium storage 嵌入在还原氧化石墨烯上的非晶碳插层 MoS2 纳米片可实现出色的高倍率和超长循环钠存储
IF 10.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-08 DOI: 10.1002/eom2.12479
Jun Xu, Junbao Jiang, Shoufu Cao, Suwan Li, Yuanming Ma, Junwei Chen, Yan Zhang, Xiaoqing Lu

MoS2 as a typical layered transition metal dichalcogenide (LTMD) has attracted considerable attention to work as sodium host materials for sodium-ion batteries (SIBs). However, it suffers from low semiconducting behavior and high Na+ diffusion barriers. Herein, intercalation of N-doped amorphous carbon (NAC) into each interlayer of the tiny MoS2 nanosheets embedded on rGO conductive network is achieved, resulting in formation of rGO@MoS2/NAC hierarchy with interoverlapped MoS2/NAC superlattices for high-performance SIBs. Attributed to intercalation of NAC, the resulting MoS2/NAC superlattices with wide MoS2 interlayer of 1.02 nm facilitates rapid Na+ insertion/extraction and accelerates reaction kinetics. Theoretical calculations uncover that the MoS2/NAC superlattices are beneficial for enhanced electron transport, decreased Na+ diffusion barrier and improved Na+ adsorption energy. The rGO@MoS2/NAC anode presents significantly improved high-rate capabilities of 228, 207, and 166 mAh g−1 at 20, 30, and 50 A g−1, respectively, compared with two control samples of pristine MoS2 and MoS2/NAC counterparts. Excellent long-term cyclability over 10 000 cycles with extremely low capacity decay is demonstrated at high current densities of 20 and 50 A g−1. Sodium-ion full cells based on the rGO@MoS2/NAC anode are also demonstrated, yielding decent cycling stability of 200 cycles at 5C. Our work provides a novel interlayer strategy to regulate electron/Na+ transport for fast-charging SIBs.

MoS2 作为一种典型的层状过渡金属二钴化物(LTMD),在钠离子电池(SIB)中作为钠宿主材料的应用引起了广泛关注。然而,它的半导体性能较低,Na+扩散障碍较高。在本文中,将掺杂 N 的无定形碳 (NAC) 插层到嵌入在 rGO 导电网络上的微小 MoS2 纳米片的每个层间,从而形成了具有 MoS2/NAC 超晶格交叠的 rGO@MoS2/NAC 层次结构,用于制造高性能 SIB。由于 NAC 的插层作用,所形成的 MoS2/NAC 超晶格具有 1.02 nm 宽的 MoS2 夹层,有利于 Na+ 的快速插入/萃取,并加快了反应动力学。理论计算发现,MoS2/NAC 超晶格有利于增强电子传输、降低 Na+ 扩散阻力和提高 Na+ 吸附能。与两个对照样品(原始 MoS2 和 MoS2/NAC 对应样品)相比,rGO@MoS2/NAC 阳极在 20、30 和 50 A g-1 电流条件下的高速率能力分别达到 228、207 和 166 mAh g-1。在 20 A g-1 和 50 A g-1 的高电流密度下,该电池具有超过 10,000 次循环的出色长期循环能力,且容量衰减极低。此外,还展示了基于 rGO@MoS2/NAC 阳极的钠离子全电池,在 5C 温度下可稳定循环 200 次。我们的工作提供了一种新颖的层间策略,可调节快速充电 SIB 的电子/Na+ 传输。
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引用次数: 0
Energy-saving hydrogen production by heteroatom modulations coupling urea electrooxidation 通过杂原子调制耦合尿素电氧化实现节能制氢
IF 10.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-30 DOI: 10.1002/eom2.12477
Shun Lu, Xingqun Zheng, Haoqi Wang, Chuan Wang, Esther Akinlabi, Ben Bin Xu, Xiaohui Yang, Qingsong Hua, Hong Liu

Developing efficient electrocatalysts with low-cost for the urea oxidation reaction (UOR) is a significant challenge in energy-saving H2 production owing to its lower thermodynamic potential. Heteroatom incorporation strategy has been proven to boost electrocatalytic activity by altering electronic structures and revealing more active sites on catalysts. Herein, nickel hydroxide nanosheets with various vanadium incorporation (Vx-Ni(OH)2) were developed through a facile hydrothermal approach. By optimizing the incorporated vanadium contents, V6-Ni(OH)2 catalyst exhibited easily accessible active sites and enhanced charge transfer with structural advantages, then assembled as the working electrode for urea-assisted H2 production. Consequently, V6-Ni(OH)2 catalyst demonstrated superior UOR activity compared with other incorporated samples with an overpotential of 1.33 V and a Tafel slope of 28.3 mV dec−1. Theoretical calculations revealed that the improved UOR activity was attributed to the potential determining step of V-Ni(OH)2, which exhibited lower energy in comparison with the pristine Ni(OH)2 and increased electronic states density near the Fermi level. Both experimental and theoretical calculations confirmed vanadium incorporation on Ni(OH)2 could modify the electronic structure of Ni(III) species, improving electrical conductivity, and optimizing the adsorption energy for key reaction intermediates. Furthermore, the crucial contribution of vanadium incorporation with optimized electronic structures to the high UOR activity of Ni(OH)2 is demonstrated.

由于尿素氧化反应(UOR)的热力学潜力较低,因此开发低成本的高效尿素氧化反应电催化剂是节能型 H2 生产中的一项重大挑战。事实证明,杂原子掺入策略可通过改变电子结构和在催化剂上发现更多活性位点来提高电催化活性。在此,通过一种简便的水热法开发出了不同钒掺杂量的氢氧化镍纳米片(Vx-Ni(OH)2)。通过优化掺入的钒含量,V6-Ni(OH)2 催化剂表现出易于获得的活性位点和增强的电荷转移,并具有结构上的优势,然后组装成工作电极用于脲辅助生产 H2。因此,与其他掺杂样品相比,V6-Ni(OH)2 催化剂表现出更高的尿素活性,过电位为 1.33 V,塔菲尔斜率为 28.3 mV dec-1。理论计算显示,UOR 活性的提高归因于 V-Ni(OH)2 的电位决定步骤,与原始 Ni(OH)2 相比,V-Ni(OH)2 的能量更低,费米级附近的电子态密度更高。实验和理论计算都证实,在 Ni(OH)2 上掺入钒可以改变 Ni(III)物种的电子结构,提高导电性,优化关键反应中间产物的吸附能。此外,还证明了掺入钒并优化电子结构对 Ni(OH)2 的高 UOR 活性的重要贡献。
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引用次数: 0
Electrically active/inert dual-function architecture enabled by screen printing grid-like SiO2 on Cu foil for ultra-long life lithium metal anodes 通过在铜箔上丝网印刷网格状二氧化硅,实现超长寿命锂金属阳极的电活性/惰性双功能结构
IF 10.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-30 DOI: 10.1002/eom2.12478
Dongdong Li, Yue He, Bin Chen, Qingyi Liu, Jun Xu, Shengchen Yang, Wen-Yong Lai

Three-dimensional (3D) current collectors (CCs) have emerged as an effective strategy to inhibit dendrites and ensure the safety of lithium (Li) metal anodes. However, existing 3D CCs are generally too heavy (typically tens of mg cm−2) or too thick (tens to hundreds of micrometers), making large-scale production and further application challenging. Additionally, the use of single-component 3D CCs, whether electrically active or inert, only exhibits limited effects on stabilizing Li anodes. Here, we present a scalable screen-printing technique for the synthesis of ultralight (~0.4 mg cm−2) and ultrathin (~0.54 μm) SiO2 grids on Cu foil to regulate both the vertical electric field and Li-ion concentration by forming an electrically active/inert dual-function architecture. This technology breaks the limitations of traditional 3D CCs in material/fabrication costs, weight, thickness and especially, scalability for large-scale fabrication. By using this dual-function architecture, our Cu@SiO2-grid CCs (~8.31 mg cm−2), which are even lighter than the original Cu-foil CCs (~8.85 mg cm−2), realize an ultra-smooth anode surface without Li dendrites, and thus leads to an ultra-long cyclic life of over 1500 h at 1 mA cm−2. The assembled Li metal batteries demonstrate excellent capacity retention of ~80% over 400 cycles at 1 C and ~ 76% over 250 cycles at 5 C, which highlight the promising 3D CCs for practical applications.

三维(3D)电流收集器(CC)已成为抑制枝晶和确保锂(Li)金属阳极安全的有效策略。然而,现有的三维集电体通常太重(通常为几十毫克厘米-2)或太厚(几十到几百微米),使得大规模生产和进一步应用面临挑战。此外,使用单组分三维 CC,无论是电活性还是惰性,对稳定锂阳极的效果都很有限。在这里,我们提出了一种可扩展的丝网印刷技术,在铜箔上合成超轻(约 0.4 mg cm-2)、超薄(约 0.54 μm)的二氧化硅网格,通过形成电活性/惰性双功能结构来调节垂直电场和锂离子浓度。这项技术打破了传统 3D CC 在材料/制造成本、重量、厚度,特别是大规模制造的可扩展性方面的限制。通过使用这种双功能结构,我们的 Cu@SiO2 网格 CCs(约 8.31 mg cm-2)比原来的 Cu 箔 CCs(约 8.85 mg cm-2)更轻,实现了没有锂枝晶的超光滑阳极表面,从而在 1 mA cm-2 电流条件下实现了超过 1500 小时的超长循环寿命。组装后的金属锂电池在 1 摄氏度条件下循环 400 次以上可保持约 80% 的容量,在 5 摄氏度条件下循环 250 次以上可保持约 76% 的容量,显示出三维 CC 在实际应用中的广阔前景。
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引用次数: 0
Solar-powered mixed-linker metal–organic frameworks for water harvesting from arid air 用于从干旱空气中收集水的太阳能混合连接剂金属有机框架
IF 10.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-23 DOI: 10.1002/eom2.12473
Xueli Yan, Fei Xue, Chunyang Zhang, Hao Peng, Jie Huang, Feng Liu, Kejian Lu, Ruizhe Wang, Jinwen Shi, Naixu Li, Wenshuai Chen, Maochang Liu

Metal–organic frameworks (MOFs) are a class of promising nanomaterials for atmospheric water harvesting (AWH), especially in arid remote areas. However, several challenges are still faced for practical applications because of the dissatisfied water adsorption/desorption properties in terms of the capability, kinetics, and stability. Herein, we report the facile synthesis of a nano-sized octahedral nitrogen-modified MOF-801 that exhibits superior solar-powered AWH performance using a custom-made device, with a state-of-the-art water harvesting ability up to 4.64LH2OkgMOFs1 from air upon 12-h test under a relative humidity (RH) of 30% and simulated sunlight irradiation. The nitrogen-modified MOF-801 with rapid sorption–desorption kinetics, uptakes 0.29gH2OgMOFs-1 of water at 30% RH within 30 min and releases 90% of the captured water within 10 min under 1-sun illumination. The success relies on N-doping-induced mixed-linkers in the form of 2,3-diaminobutanedioic acid and fumaric acid in the unique pore structures of the MOFs for rapid and high-capacity water capture. The N-doped MOF-801 with water uptake capacity, fast adsorption kinetics, and cycle stability sheds light on the practical use of MOFs for effective solar-powered water harvesting from droughty air.

金属有机框架(MOFs)是一类很有前景的大气集水(AWH)纳米材料,尤其适用于干旱偏远地区。然而,由于MOFs在吸附/解吸水能力、动力学和稳定性等方面的特性不尽人意,其实际应用仍面临一些挑战。在此,我们报告了一种纳米级八面体氮修饰 MOF-801的简易合成方法,该方法利用定制的装置表现出了卓越的太阳能供电 AWH 性能,其最先进的集水能力可达 4.64LH2OkgMOFs-1$$ 4.64kern0.5em {mathrm{L}}_{{mmathrm{H}}_2mathrm{O}}kern0.5em {{mathrm{kg}}_{{mmathrm{MOFs}}^{-1}$$ 在相对湿度(RH)为 30% 和模拟太阳光照射下进行 12 小时测试后,MOF-801 从空气中收集的水量达到 4.64LH2OkgMOFs-1$$ 4.64kern0.5em {mathrm{L}}_{{mmathrm{H}}_2mathrm{O}}kern0.5em {{mathrm{kg}}_{{mmathrm{MOFs}}^{-1}$$氮修饰的 MOF-801 具有快速的吸附-解吸动力学,在 30% 的相对湿度(RH)和模拟太阳光照射条件下,从空气中吸收 0.29gH2OgMOFs-1$$ 0.29kern0.5em {mathrm{g}}_{{mathrm{H}}_2mathrm{O}}kern0.5em {{mathrm{g}}_{mathrm{MOFs}}^{hbox{-}1}$ 在 30% 相对湿度下,30 分钟内释放出 90% 的水,在 1 个太阳光照射下,10 分钟内释放出 90% 的捕获水。这一成功依赖于 MOF 独特的孔隙结构中以 2,3-二氨基丁二酸和富马酸形式存在的 N 掺杂诱导混合连接体,从而实现了快速、高容量的水捕获。掺杂了 N 的 MOF-801 具有吸水能力、快速吸附动力学和循环稳定性,这为实际利用 MOFs 从干旱空气中有效收集太阳能水提供了启示。
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引用次数: 0
Unlocking fast-charging capabilities of lithium-ion batteries through liquid electrolyte engineering 通过液态电解质工程释放锂离子电池的快速充电能力
IF 10.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-20 DOI: 10.1002/eom2.12476
Chaeeun Song, Seung Hee Han, Hyeongyu Moon, Nam-Soon Choi

Global trends toward green energy have empowered the extensive application of high-performance energy storage systems. With the worldwide spread of electric vehicles (EVs), lithium-ion batteries (LIBs) capable of fast-charging have become increasingly important. Nonetheless, state-of-the-art LIBs have failed to satisfy the demands of prospective customers, including rapid charging, extended cycle life, and high energy density. Addressing these challenges through innovations in material science and other advanced battery technologies is essential for meeting the growing demands of prospective customers. Besides the choice of active materials, electrolyte formulation has a significant impact on the fast-charging performance and cycle life of LIBs over a wide range of temperatures. The liquid electrolyte is typically composed of lithium salts to provide an ion source, solvents to carry Li+ ions, and functional additives to build a stable solid electrolyte interphase (SEI). To enable the fast movement of Li+ ions, the liquid electrolytes should have low viscosity and high ionic conductivity. Meanwhile, SEI layers must be thin, uniform and ionically conductive. Furthermore, the low binding energy of the solvent facilitates desolvation of the solvation sheath, enabling fast Li+ ion transport to the anode during fast charging. This review provides the latest insights into rapid Li+ ion transport during fast charging, focusing on ensuring a deeper understanding of liquid electrolyte chemistry. The involvement of existing electrolyte mechanisms in materials discovery will develop electrolyte engineering techniques to improve the fast-charging performance of batteries over a wide temperature range and will also facilitate the development of EV-adoptable advanced electrodes.

全球绿色能源的发展趋势推动了高性能储能系统的广泛应用。随着电动汽车(EV)在全球的普及,能够快速充电的锂离子电池(LIB)变得越来越重要。然而,最先进的锂离子电池无法满足潜在客户的需求,包括快速充电、延长循环寿命和高能量密度。要满足潜在客户日益增长的需求,就必须通过材料科学和其他先进电池技术的创新来应对这些挑战。除了活性材料的选择,电解质配方对液态电解质电池在各种温度下的快速充电性能和循环寿命也有重大影响。液态电解质通常由提供离子源的锂盐、携带 Li+ 离子的溶剂和构建稳定固态电解质相(SEI)的功能添加剂组成。为使 Li+ 离子快速移动,液态电解质应具有低粘度和高离子电导率。同时,SEI 层必须薄、均匀且具有离子导电性。此外,溶剂的低结合能可促进溶解鞘的解溶,从而在快速充电过程中将 Li+ 离子快速输送到阳极。本综述提供了快速充电过程中 Li+ 离子快速传输的最新见解,重点是确保加深对液态电解质化学的理解。将现有的电解质机理应用于材料发现,将有助于开发电解质工程技术,从而提高电池在宽温度范围内的快速充电性能,同时也将促进可应用于电动汽车的先进电极的开发。
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引用次数: 0
Textile-based triboelectric nanogenerators integrated with 2D materials 与二维材料集成的纺织品基三电纳米发电机
IF 10.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-18 DOI: 10.1002/eom2.12471
Iftikhar Ali, Nazmul Karim, Shaila Afroj

The human body continuously generates ambient mechanical energy through diverse movements, such as walking and cycling, which can be harvested via various renewable energy harvesting mechanisms. Triboelectric Nanogenerator (TENG) stands out as one of the most promising emerging renewable energy harvesting technologies for wearable applications due to its ability to harness various forms of mechanical energies, including vibrations, pressure, and rotations, and convert them into electricity. However, their application is limited due to challenges in achieving performance, flexibility, low power consumption, and durability. Here, we present a robust and high-performance self-powered system integrated into cotton fabric by incorporating a textile-based triboelectric nanogenerator (T-TENG) based on 2D materials, addressing both energy harvesting and storage. The proposed system extracts significant ambient mechanical energy from human body movements and stores it in a textile supercapacitor (T-Supercap). The integration of 2D materials (graphene and MoS2) in fabrication enhances the performance of T-TENG significantly, as demonstrated by a record-high open-circuit voltage of 1068 V and a power density of 14.64 W/m2 under a force of 22 N. The developed T-TENG in this study effectively powers 200+ LEDs and a miniature watch while also charging the T-Supercap with 4-5 N force for efficient miniature electronics operation. Integrated as a step counter within a sock, the T-TENG serves as a self-powered step counter sensor. This work establishes a promising platform for wearable electronic textiles, contributing significantly to the advancement of sustainable and autonomous self-powered wearable technologies.

人体通过行走和骑自行车等各种运动不断产生环境机械能,这些机械能可以通过各种可再生能源收集机制收集。三电纳米发电机(TENG)能够利用各种形式的机械能,包括振动、压力和旋转,并将其转化为电能,因此是可穿戴应用中最有前途的新兴可再生能源采集技术之一。然而,由于在实现性能、灵活性、低功耗和耐用性方面存在挑战,其应用受到了限制。在这里,我们介绍了一种将基于二维材料的纺织品三电纳米发电机(T-TENG)集成到棉织物中的坚固耐用的高性能自供电系统,同时解决了能量收集和存储问题。所提议的系统可从人体运动中提取大量环境机械能,并将其储存在纺织品超级电容器(T-Supercap)中。二维材料(石墨烯和 MoS2)的集成制造大大提高了 T-TENG 的性能,其开路电压达到创纪录的 1068 V,在 22 N 的力下功率密度达到 14.64 W/m2。本研究中开发的 T-TENG 能有效地为 200 多个 LED 和一块微型手表供电,同时还能以 4-5 N 的力为 T 型超级电容器充电,从而实现微型电子产品的高效运行。T-TENG 将计步器集成在袜子中,可作为自供电的计步传感器。这项工作为可穿戴电子纺织品建立了一个前景广阔的平台,为可持续和自主自供电可穿戴技术的发展做出了重大贡献。
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引用次数: 0
Two-dimensionalization of 3D perovskites for passive narrowband Photodetection 用于无源窄带光电探测的三维过氧化物的二维化
IF 10.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-17 DOI: 10.1002/eom2.12472
Xin Song, Siwen Liu, Lizhi Ren, Yunxian Zuo, Shimin Wang, Erjing Wang, Jin Qian, Tao Ye, Kai Wang, Congcong Wu

In the rapidly advancing field of information technology, passive sensors with the exemption of external power input can serve as intelligent instruments for end-node data acquisition. 3D perovskites have been recognized as a superior optoelectronic material but suffering from notorious instability due to their “soft lattice” nature. Replacing by their 2D counterparts in these photo-sensing applications can boost the reliability level. However, traditional fabrication for 2D perovskite relay on wet chemistry methods, exhibiting complication, and inefficiency in making high-quality films for device integration. This study unveils a new solid–solid conversion routing toward a direct transformation from 3D orientated films into 2D highly crystalline configuration, based on a spontaneous lattice regulation mechanism through an amine steam treatment. The resultant 2D film exhibits greater orientational micromorphology and a distinct monochromatic narrowband light sensing behavior after integration into a self-powered photodetector. This method on perovskite conversion bears the promise of advanced future-manufacturing for high-performance photonic sensing.

在飞速发展的信息技术领域,无需外部电源输入的无源传感器可作为终端节点数据采集的智能仪器。三维过氧化物已被公认为一种优质光电材料,但由于其 "软晶格 "性质,其不稳定性也是众所周知的。在这些光传感应用中,用二维对应材料取而代之可以提高可靠性水平。然而,传统的二维包晶制造方法依赖于湿化学方法,在制造用于设备集成的高质量薄膜方面表现出复杂性和低效率。本研究揭示了一种新的固-固转换路线,通过胺蒸汽处理,基于自发晶格调节机制,将三维定向薄膜直接转化为二维高结晶构造。由此产生的二维薄膜在集成到自供电光电探测器后,显示出更大的取向微观形态和独特的单色窄带光传感性能。这种包晶石转换方法有望在未来实现高性能光子传感的先进制造。
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引用次数: 0
Back cover Image 封底图片
Q1 Chemistry Pub Date : 2024-06-17 DOI: 10.1002/eom2.12475

This illustration depicts the precise carbon coating of a cost-effective SiO2 primary particle using different organic materials to create a highly electronic conductive material. This development enhances high-energy-density lithium-ion battery systems, making them ideal for electric vehicle applications by improving performance, and affordability.

该插图描述了利用不同的有机材料对具有成本效益的二氧化硅初级粒子进行精确的碳涂层,从而制造出一种高电子导电材料。这一研发成果增强了高能量密度锂离子电池系统,通过提高性能和经济性,使其成为电动汽车应用的理想选择。
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引用次数: 0
Front cover Image 封面图片
Q1 Chemistry Pub Date : 2024-06-17 DOI: 10.1002/eom2.12370

The cover image of the publication eom2.12453 showed how lignin, a bio-polymer material, significantly enhances the sensitivity of MXene composite as a 2D materials chemiresistive sensor for molecular gas detection. This study also demonstrated a hybridized MXene composite flexible chemiresistive sensor, which paves the way for new solid-state sensing platforms for curvature structures.

刊物 eom2.12453 的封面图片展示了木质素(一种生物聚合物材料)如何显著提高 MXene 复合材料作为二维材料化学电阻传感器用于分子气体检测的灵敏度。这项研究还展示了一种杂化 MXene 复合材料柔性化学电阻传感器,为曲率结构的新型固态传感平台铺平了道路。
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引用次数: 0
Inside Front Cover Image 封面内页图片
Q1 Chemistry Pub Date : 2024-06-17 DOI: 10.1002/eom2.12474

Indoor photovoltaics suffer from non-radiative recombination and parasitic leakage current especially due to low carrier density. Incorporating a porous alumina interlayer in perovskite photovoltaics mitigates non-radiative recombination and parasitic leakage current, enhancing efficiency under low-light indoor conditions. This strategy is demonstrated in large-area modules at 23.03 cm2, achieving 33.5% efficiency and 107.3 µW/cm2 power density under LED 1000 lux.

由于载流子密度较低,室内光伏技术尤其受到非辐射重组和寄生漏电流的影响。在过氧化物光伏中加入多孔氧化铝中间层可减轻非辐射重组和寄生漏电流,提高室内弱光条件下的效率。在 23.03 平方厘米的大面积模块中演示了这一策略,在 LED 1000 勒克斯条件下实现了 33.5% 的效率和 107.3 µW/cm2 的功率密度。
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引用次数: 0
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