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Substituent engineering in tertiary phosphine oxides for passivating defects of perovskite solar cells 用于钝化过氧化物太阳能电池缺陷的叔膦氧化物取代基工程
IF 10.7 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-17 DOI: 10.1002/eom2.12470
Sun-Ho Lee, Seong Chan Cho, Sang Uck Lee, Nam-Gyu Park

Defect passivation based on Lewis acid–base chemistry has been regarded as an effective strategy to improve the photovoltaic performance and stability of perovskite solar cells (PSCs). Here, we report on tertiary phosphine oxides (R3PO) as materials for defect passivation, where photovoltaic performance was investigated depending on the substituents R. Electron-donating ability of the substituents in R3PO was found to play an important role in passivation. Cyclohexyl substituent was better in achieving photovoltaic performance than linear hexyl substituent. The heterocyclic morpholine substituent bearing oxygen and nitrogen in cyclohexyl form further improved photovoltaic performance due to its enhanced electron-donating ability. Compared with an untreated PSC, the trimorpholinophosphine oxide (TMPPO)-treated PSC improved the power conversion efficiency from 21.95% to 23.72%. Additionally, the dark-storage stability test with an unencapsulated device showed that the TMPPO-treated device maintained 92.7% of its initial PCE after 1250 h, while 86.8% was maintained for the untreated device. Three hundred hour-light-soaking of the encapsulated devices revealed that the operational stability of the TMPPO-treated PSC was superior to the untreated device.

基于路易斯酸碱化学的缺陷钝化被认为是提高过氧化物太阳能电池(PSCs)光电性能和稳定性的有效策略。在此,我们报告了作为缺陷钝化材料的叔膦氧化物(R3PO),并根据取代基 R 的不同对其光伏性能进行了研究。在实现光伏性能方面,环己基取代基比直链己基取代基更好。环己基形式的杂环吗啉取代基中含有氧和氮,由于其电子负载能力增强,可进一步提高光伏性能。与未经处理的 PSC 相比,经过三吗啉氧化膦 (TMPPO) 处理的 PSC 可将功率转换效率从 21.95% 提高到 23.72%。此外,未封装器件的黑暗储存稳定性测试表明,经 TMPPO 处理的器件在 1250 小时后仍能保持 92.7% 的初始 PCE,而未经处理的器件则能保持 86.8%。对封装装置进行三百小时的光照浸泡表明,经 TMPPO 处理的 PSC 的操作稳定性优于未经处理的装置。
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引用次数: 0
Precision integration of uniform molecular-level carbon into porous silica framework for synergistic electrochemical activation in high-performance lithium–ion batteries 将均匀的分子级碳精确集成到多孔二氧化硅框架中,为高性能锂离子电池提供协同电化学活化功能
Q1 Chemistry Pub Date : 2024-06-12 DOI: 10.1002/eom2.12469
Seungbae Oh, Xue Dong, Chaeheon Woo, Xiaojie Zhang, Yeongjin Kim, Kyung Hwan Choi, Bom Lee, Ji-Hee Kim, Jinsu Kang, Hyeon-Seok Bang, Jiho Jeon, Hyung-Suk Oh, Hak Ki Yu, Junyoung Mun, Jae-Young Choi

The development of advanced anode materials for lithium-ion batteries that can provide high specific capacity and stable cycle performance is of paramount importance. This study presents a novel approach for synthesizing molecular-level homogeneous carbon integration to porous SiO2 nanoparticles (SiO2@C NPs) tailored to enhance their electrochemical activities for lithium-ion battery anode. By varying the ratio of the precursors for sol–gel reaction of (phenyltrimethoxysilane (PTMS) and tetraethoxysilane (TEOS)), the carbon content and porosity within SiO2@C NPs is precisely controlled. With a 4:6 PTMS and TEOS ratio, the SiO2@C NPs exhibit a highly mesoporous structure with thin carbon and the partially reduced SiOx phases, which balances ion and charge transfer for electrochemical activation of SiO2@C NPs resulting remarkable capacity and cycle performance. This study offers a novel strategy for preparing affordable high capacity SiO2-based advanced anode materials with enhanced electrochemical performances.

开发可提供高比容量和稳定循环性能的先进锂离子电池负极材料至关重要。本研究提出了一种新方法,用于合成分子级同质碳与多孔二氧化硅纳米颗粒(SiO2@C NPs)的整合,以提高其在锂离子电池负极中的电化学活性。通过改变溶胶-凝胶反应前驱体(苯基三甲氧基硅烷(PTMS)和四乙氧基硅烷(TEOS))的比例,可以精确控制 SiO2@C NPs 中的碳含量和孔隙率。当 PTMS 和 TEOS 的比例为 4:6 时,SiO2@C NPs 呈现出具有薄碳和部分还原 SiOx 相的高度介孔结构,从而平衡了 SiO2@C NPs 电化学活化过程中的离子和电荷转移,使其具有显著的容量和循环性能。这项研究为制备经济实惠、电化学性能更强的高容量 SiO2 基先进正极材料提供了一种新策略。
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引用次数: 0
Controlled growth of uniform and dense perovskite layers on SnO2 via interface passivation by PbS quantum dots 通过 PbS 量子点的界面钝化,在 SnO2 上控制生长均匀致密的过氧化物层
Q1 Chemistry Pub Date : 2024-06-03 DOI: 10.1002/eom2.12456
Yulin Liu, Sumin Bae, Seongha Lee, Anqi Wang, Youngsoo Jung, Doh-Kwon Lee, Jung-Kun Lee

Formamidinium lead iodide (FAPbI3) and SnO2 are a promising pair of halide perovskite and electron transport layer (ETL). However, FAPbI3 and SnO2 have inherent problems such as high crystallization temperature of FAPbI3 and surface defects of SnO2 like oxygen vacancies. They cause low crystallinity, non-uniform grain growth, and more interface defects, leading to carrier recombination and leakage current. The passivation of the interface between FAPbI3 and SnO2 is an effective process to address these materials issues. Herein, a dual role of lead sulfide (PbS) quantum dots (QDs) in the interface passivation is explored. PbS QDs which are introduced to the interface between FAPbI3 and ETL, link to Sn-dangling bonds of SnO2 ETLs and anchor the iodine atoms of FAPbI3. This changes considerably lower nonradiative recombination, achieve a better energetic alignment between ETL and PbI3, and facilitate electron extraction, leading to a power conversion efficiency of 21.66%.

碘化甲脒铅(FAPbI3)和二氧化锡是一对很有前途的卤化物包晶和电子传输层(ETL)。然而,FAPbI3 和 SnO2 都存在固有的问题,例如 FAPbI3 的结晶温度较高,而 SnO2 则存在氧空位等表面缺陷。它们会造成结晶度低、晶粒生长不均匀和更多的界面缺陷,从而导致载流子重组和泄漏电流。对 FAPbI3 和 SnO2 之间的界面进行钝化是解决这些材料问题的有效方法。本文探讨了硫化铅(PbS)量子点(QDs)在界面钝化中的双重作用。硫化铅量子点被引入 FAPbI3 和 ETL 之间的界面,与二氧化锡 ETL 的锡键相连,并锚定 FAPbI3 的碘原子。这种变化大大降低了非辐射重组,实现了 ETL 和 PbI3 之间更好的能量排列,并促进了电子萃取,从而使功率转换效率达到 21.66%。
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引用次数: 0
Mitigation of parasitic leakage current in indoor perovskite photovoltaic modules using porous alumina interlayer 利用多孔氧化铝中间膜缓解室内过氧化物光伏组件中的寄生漏电流
Q1 Chemistry Pub Date : 2024-05-29 DOI: 10.1002/eom2.12455
Gyeong G. Jeon, Da Seul Lee, Min Jun Choi, You-Hyun Seo, Shujuan Huang, Jong H. Kim, Seong Sik Shin, Jincheol Kim

Indoor photovoltaics are limited by their inherently low-photogenerated carrier density, leading to heightened carrier recombination and adverse leakage currents compared with conventional solar cells operating under 1 sun condition. To address these problems, this work incorporates a porous insulating interlayer (Al2O3) in perovskite devices, which effectively mitigates recombination and parasitic leakage current. A systematic investigation of the relationship between shunt resistance, photocarrier generation, and recombination at different light intensities demonstrates the effectiveness of the alumina interlayer in perovskite solar cells under low-light conditions. Moreover, the practicability of the alumina interlayer was demonstrated through its successful implementation in a large-area perovskite solar module (PSM). With bandgap engineering, the optimized PSM achieves a remarkable power conversion efficiency of 33.5% and a record-breaking power density of 107.3 μW cm−2 under 1000 lux illumination. These results underscore the potential of alumina interlayers in improving energy harvesting performance, particularly in low-light indoor environments.

室内光伏技术因其固有的低光生载流子密度而受到限制,与在日照条件下工作的传统太阳能电池相比,室内光伏技术会导致载流子高度重组和不利的漏电流。为了解决这些问题,这项研究在过氧化物设备中加入了多孔绝缘中间层(Al2O3),从而有效地缓解了载流子重组和寄生漏电流。对不同光照强度下并联电阻、光载流子生成和重组之间关系的系统研究表明,氧化铝中间膜在低光照条件下的包晶体太阳能电池中非常有效。此外,氧化铝中间膜在大面积透辉石太阳能模块(PSM)中的成功应用也证明了它的实用性。通过带隙工程,优化后的 PSM 在 1000 勒克斯照明条件下实现了 33.5% 的出色功率转换效率和 107.3 μW cm-2 的破纪录功率密度。这些结果凸显了氧化铝夹层在提高能量收集性能方面的潜力,尤其是在室内弱光环境下。
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引用次数: 0
Reinforced nanowrinkle electrospun photothermal membranes via solvent-induced recrystallization 通过溶剂诱导再结晶强化纳米皱纹电纺光热膜
Q1 Chemistry Pub Date : 2024-05-19 DOI: 10.1002/eom2.12454
Jinlin Chang, Weiling Wang, Zhaoxin Li, Yujiao Wang, Yacong Hou, Zhiyuan Cao, Zhenwei Liang, Yuan Ma, Ding Weng, Jun Song, Yadong Yu, Lei Chen, Jiadao Wang

Wearable photothermal materials can capture light energy in nature and convert it into heat energy, which is critical for flexible outdoor sports. However, the conventional flexible photothermal membranes with low specific surface area restrict the maximum photothermal capability, and loose structure of electrospun membrane limits durability of wearable materials. Here, an ultrathin nanostructure candle soot/multi-walled carbon nanotubes/poly (L-lactic acid) (CS/MWCNTs/PLLA) photothermal membrane is first prepared via solvent-induced recrystallization. The white blood cell membrane-like nanowrinkles with high specific surface area are achieved for the first time and exhibit optimal light absorption. The solvent-induced recrystallization also enables the membrane to realize large strength and durability. Meanwhile, the membranes also show two-sided heterochromatic features and transparency in thick and thin situations, respectively, suggesting outstanding fashionability. The nano-wrinkled photothermal membranes by novel solvent-induced recrystallization show high flexibility, fashionability, strength, and photothermal characteristics, which have huge potential for outdoor warmth and winter sportswear.

可穿戴光热材料能够捕捉自然界中的光能并将其转化为热能,这对于柔性户外运动至关重要。然而,传统的柔性光热膜比表面积低,限制了光热能力的最大化,而电纺膜结构松散,限制了可穿戴材料的耐用性。本文首先通过溶剂诱导重结晶法制备了超薄纳米结构烛烟/多壁碳纳米管/聚(L-乳酸)(CS/MWCNTs/PLLA)光热膜。首次实现了具有高比表面积的白细胞膜状纳米皱纹,并表现出最佳的光吸收性能。溶剂诱导重结晶还使膜具有高强度和耐久性。同时,该膜还呈现出双面异色特征,并在厚膜和薄膜的情况下分别呈现出透明性,显示出卓越的时尚性。通过新型溶剂诱导重结晶技术制备的纳米皱纹光热膜具有高柔韧性、时尚性、强度和光热特性,在户外保暖和冬季运动服方面具有巨大潜力。
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引用次数: 0
Enhanced sensitivity of zero-bias-operated MXene chemiresistive sensor via lignin hybridization 通过木质素杂交提高零偏压操作 MXene 化学电阻传感器的灵敏度
Q1 Chemistry Pub Date : 2024-05-07 DOI: 10.1002/eom2.12453
I Ketut Gary Devara, Mi Ji Kwon, Su-Yeon Cho, Dong-Jun Kwon, Jun Hong Park

As global urbanization intensifies, there is an increasing need for highly sensitive and accurate environmental monitoring devices that can meet the demands of specific gas sensing applications with low power consumption. This study focuses on enhancing the sensitivity of MXene-based chemiresistive sensors for detecting CO2(g) and NO2(g) under zero-bias operation. This study shows that lignin hybridization effectively improves the sensitivity of a Ti3C2Tx MXene-based chemiresistive sensor; under zero-bias operation, lignin hybridization increases the sensitivity to 15 ppm NO2(g) and CO2(g) by 157.38% and 297.95%, respectively. When deposited on a flexible substrate, the MXene/lignin flexible sensor shows a similar response and sensitivity to 15 ppm NO2(g) and CO2(g) under 38° curvature compared to the planar sensor. Consequently, the MXene/lignin hybrid sensor is attractive for room temperature and zero-bias NO2(g) and CO2(g) detection. The MXene/lignin flexible sensor serves as a model system for advanced solid-state sensory platforms suitable for curved structures.

随着全球城市化进程的加剧,人们越来越需要高灵敏度和精确的环境监测设备,以满足特定气体传感应用对低功耗的要求。本研究的重点是提高基于 MXene 的化学电阻传感器在零偏压工作条件下检测 CO2(g) 和 NO2(g) 的灵敏度。研究表明,木质素杂化可有效提高 Ti3C2Tx MXene 基化学电阻传感器的灵敏度;在零偏置工作条件下,木质素杂化可将 15 ppm NO2(g) 和 CO2(g) 的灵敏度分别提高 157.38% 和 297.95%。当沉积在柔性基底上时,与平面传感器相比,MXene/木质素柔性传感器在 38° 曲度下对 15 ppm NO2(g) 和 CO2(g) 的响应和灵敏度相似。因此,MXene/木质素混合传感器在室温零偏差检测二氧化氮(g)和二氧化碳(g)方面具有吸引力。MXene/lignin 柔性传感器可作为适用于曲面结构的先进固态传感平台的模型系统。
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引用次数: 0
A carbon dot toolbox for managing biotic and abiotic stresses in crop production systems 管理作物生产系统中生物和非生物压力的碳点工具箱
Q1 Chemistry Pub Date : 2024-05-05 DOI: 10.1002/eom2.12451
Muhammad U. Zia, Prabhakaran Thanjavur Sambasivam, Dechao Chen, Shamsul A. Bhuiyan, Rebecca Ford, Qin Li

The productivity of global crop production is under threat caused by various biotic and abiotic adverse conditions, such as plant diseases and pests, which are responsible for 20%–40% of global crop losses estimated at a value of USD 220 billion, and can be further exacerbated by climate change. Agricultural industries are calling for game-changer technologies to enable productive and sustainable farming. Carbon dots (C-dots) are carbon-based nanoparticles, smaller than 50 nm, exhibiting unique opto-electro-properties. They have been shown to have positive impact on managing diverse biotic and abiotic stresses faced by the crops. Owing to their versatile carbon chemistry, the surface functionalities of C-dots can be readily tuned to regulate plant physiological processes. This review is focussed on establishing the correlations between the physiochemical properties of C-dots and their impacts on plants growth and health. The summary of the literature demonstrates that C-dots hold great promise in improving plant tolerance to heat, drought, toxic chemicals, and invading pathogens.

全球作物生产的生产力正受到植物病虫害等各种生物和非生物不利条件的威胁,这些不利条件造成的损失占全球作物损失的 20%-40%,估计价值达 2200 亿美元,气候变化还会进一步加剧这种威胁。农业产业正在呼唤改变游戏规则的技术,以实现高产和可持续的耕作。碳点(C-dots)是小于 50 纳米的碳基纳米粒子,具有独特的光电特性。研究表明,它们对管理作物面临的各种生物和非生物压力具有积极影响。由于碳化学性质多变,C-点的表面功能可随时调整,以调节植物的生理过程。本综述的重点是建立 C 点的理化特性与其对植物生长和健康的影响之间的相关性。文献总结表明,C-点在提高植物对高温、干旱、有毒化学品和病原体入侵的耐受性方面大有可为。
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引用次数: 0
Phosphorus-based anodes for fast-charging alkali metal ion batteries 用于快速充电碱金属离子电池的磷基阳极
Q1 Chemistry Pub Date : 2024-05-04 DOI: 10.1002/eom2.12452
Xuexia Lan, Zhen Li, Yi Zeng, Cuiping Han, Jing Peng, Hui-Ming Cheng

Advancing fast-charging technology is an important strategy for the development of alkali metal ion batteries (AMIBs). The exploitation of a new generation of anode material system with high-rate performance, high capacity, and low risk of lithium/sodium/potassium plating is critical to realize fast-charging capability of AMIBs while maintaining high energy density and safety. Among them, phosphorus-based anodes including phosphorus anodes and metal phosphide anodes have attracted wide attention, due to their high theoretical capacities, safe reaction voltages, and natural abundance. In this review, we summarize the research progress of different phosphorus-based anodes for fast-charging AMIBs, including material properties, mechanisms for storing alkali metal ions, key challenges and solution strategies for achieving fast-charging capability. Moreover, the future development directions of phosphorus-based anodes in fast-charging AMIBs are highlighted.

推进快速充电技术是碱金属离子电池(AMIB)发展的重要战略。要在保持高能量密度和安全性的前提下实现碱金属离子电池的快速充电能力,开发具有高倍率性能、高容量和低锂/钠/钾电镀风险的新一代负极材料体系至关重要。其中,磷基阳极(包括磷阳极和金属磷化物阳极)因其理论容量高、反应电压安全、天然丰富而受到广泛关注。在这篇综述中,我们总结了用于快速充电 AMIB 的不同磷基阳极的研究进展,包括材料特性、碱金属离子存储机理、实现快速充电能力的关键挑战和解决策略。此外,还强调了磷基阳极在快速充电 AMIB 中的未来发展方向。
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引用次数: 0
AIoT-enhanced health management system using soft and stretchable triboelectric sensors for human behavior monitoring 使用用于人类行为监测的软质可拉伸三电传感器的人工智能物联网增强型健康管理系统
Q1 Chemistry Pub Date : 2024-05-02 DOI: 10.1002/eom2.12448
Liang Xu, Songyi Zhong, Tao Yue, Zixuan Zhang, Xiao Lu, Yangqiao Lin, Long Li, Yingzhong Tian, Tao Jin, Quan Zhang, Chengkuo Lee

Sedentary, inadequate sleep and exercise can affect human health. Artificial intelligence (AI) and Internet of Things (IoT) create the Artificial Intelligence of Things (AIoT), providing the possibility to solve these problems. This paper presents a novel approach to monitor various human behaviors for AIoT-based health management using triboelectric nanogenerator (TENG) sensors. The insole with solely one TENG sensor, creating a most simplified system that utilizes machine learning (ML) for personalized motion monitoring, encompassing identity recognition and gait classification. A cushion with 12 TENG sensors achieves real-time identity and sitting posture recognition with accuracy rates of 98.86% and 98.40%, respectively, effectively correcting sedentary behavior. Similarly, a smart pillow, equipped with 15 sensory channels, detects head movements during sleep, identifying 8 sleep patterns with 96.25% accuracy. Ultimately, constructing an AIoT-based health management system to analyze these data, displaying health status through human-machine interfaces, offers the potential to help individuals maintain good health.

久坐不动、睡眠不足和运动不足都会影响人体健康。人工智能(AI)和物联网(IoT)创造了人工智能物联网(AIoT),为解决这些问题提供了可能。本文介绍了一种利用三电纳米发电机(TENG)传感器监测各种人体行为的新方法,以实现基于 AIoT 的健康管理。鞋垫只配备了一个 TENG 传感器,创造了一个最简化的系统,利用机器学习(ML)进行个性化运动监测,包括身份识别和步态分类。配备 12 个 TENG 传感器的坐垫可实现实时身份和坐姿识别,准确率分别达到 98.86% 和 98.40%,有效纠正久坐行为。同样,配备 15 个传感通道的智能枕头可检测睡眠时的头部运动,识别出 8 种睡眠模式,准确率达 96.25%。最终,构建一个基于人工智能物联网的健康管理系统来分析这些数据,通过人机界面显示健康状况,有望帮助个人保持身体健康。
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引用次数: 0
Life cycle assessment of lead-free potassium sodium niobate versus lead zirconate titanate: Energy and environmental impacts 无铅铌酸钠钾与锆钛酸铅的生命周期评估:能源和环境影响
Q1 Chemistry Pub Date : 2024-04-25 DOI: 10.1002/eom2.12450
Yanqi Wu, Pak-Sheng Soon, Jing-Tong Lu, Jinling Zhou, Yi-Xuan Liu, Zhaohui Guo, Ke Wang, Wen Gong

Over the years, lead-based piezoelectric ceramics found extensive use in vital fields such as sensors and actuators. Despite their exceptional electromechanical properties, lead-containing materials pose severe environmental risks and foster a new era of lead-free piezoelectric materials after decades of research. However, recent comparative assessments of potassium sodium niobate (KNN) versus lead zirconate titanate (PZT) piezoelectric materials proposed that the environmental damage already presented before use due to raw material extraction and processing, invoking concerns on the true greenness of the lead-free alternatives. Nevertheless, many other factors deserve further consideration, for example, reference geometry and life cycle stage. Herein, the comprehensive life cycle assessment is undertaken on PZT and KNN-based ceramics with a unit volume of 0.001 m3 from cradle to gate. Results show that PZT exhibits higher negative impacts than KNN-based counterparts, attributed to lead extraction, processing, and associated environmental emissions. Across primary quantitative impact indicators from toxicity, environmental, and resource aspects, KNN-based ceramics impose fewer risks on the environment and human health, with the overall impact being only 28% of PZT ceramics. Still, more efficient methods are required for KNN-based ceramics to reduce the high energy consumption and emission during extraction and purification of raw material Nb2O5. This work not only offers critical insights for material development but also serves as a multifaceted reference for advanced fabrication technologies.

多年来,铅基压电陶瓷被广泛应用于传感器和致动器等重要领域。尽管含铅材料具有卓越的机电特性,但它会带来严重的环境风险,因此经过数十年的研究,无铅压电材料的新时代已经到来。然而,最近对铌酸钠钾(KNN)和锆钛酸铅(PZT)压电材料进行的比较评估表明,由于原材料的提取和加工,在使用前就已经对环境造成了破坏,这引发了人们对无铅替代品是否真正绿色环保的担忧。不过,还有许多其他因素值得进一步考虑,例如参考几何形状和生命周期阶段。在此,我们对单位体积为 0.001 立方米的 PZT 和 KNN 基陶瓷进行了从摇篮到大门的全面生命周期评估。结果表明,与 KNN 基陶瓷相比,PZT 具有更高的负面影响,主要归因于铅的提取、加工和相关的环境排放。从毒性、环境和资源方面的主要定量影响指标来看,KNN 基陶瓷对环境和人类健康造成的风险较小,总体影响仅为 PZT 陶瓷的 28%。尽管如此,KNN 基陶瓷仍需要更有效的方法,以减少原材料 Nb2O5 的提取和提纯过程中的高能耗和高排放。这项工作不仅为材料开发提供了重要启示,也为先进的制造技术提供了多方面的参考。
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引用次数: 0
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