ACS Materials Letters最新文献_第6页

Understanding Direct-Ammonia Protonic Ceramic Fuel Cells: High-Performance in the Absence of Precious Metal Catalysts 了解直接氨质子陶瓷燃料电池：在不使用贵金属催化剂的情况下实现高性能

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-24 DOI: 10.1021/acsenergylett.4c0226310.1021/acsenergylett.4c02263

Jiwon Yun, Grace Xiong, Seungchan Kim, Dylan Bardgett, Sihyuk Choi* and Sossina M. Haile*,

{"title":"Understanding Direct-Ammonia Protonic Ceramic Fuel Cells: High-Performance in the Absence of Precious Metal Catalysts","authors":"Jiwon Yun, Grace Xiong, Seungchan Kim, Dylan Bardgett, Sihyuk Choi* and Sossina M. Haile*, ","doi":"10.1021/acsenergylett.4c0226310.1021/acsenergylett.4c02263","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02263https://doi.org/10.1021/acsenergylett.4c02263","url":null,"abstract":"Ammonia has received considerable attention as a promising carbon-free hydrogen carrier. At temperatures above 400 °C, NH3 is thermodynamically unstable with respect to decomposition into nitrogen and hydrogen and is, thus, suitable for direct use in solid oxide fuel cells (SOFCs) without external reforming. However, poor catalytic activity for ammonia decomposition at the moderate temperatures of protonic ceramic fuel cell (PCFC) operation has resulted in low fuel cell power output relative to operation on hydrogen and likely contributes to reported cell degradation. Here we prepared cells based on a thermodynamically robust electrolyte, a high activity cathode, and an anode with a distinctive structure to overcome challenges of poor activity and stability. The cells delivered peak power densities of 0.59 and 0.44 W cm–2 under H2 and NH3, respectively, at 500 °C, excellent stability over a period of 200 h, and no detectable NOx in the anode exhaust gas.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5520–5528 5520–5528"},"PeriodicalIF":19.3,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608746","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dehydration Conditions and Ultrafast Rehydration of Prussian White: Phase Transition Dynamics and Implications for Sodium-Ion Batteries. 普鲁士白的脱水条件和超快再水化：相变动力学及其对钠离子电池的影响。

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2024-10-24 eCollection Date: 2024-11-04 DOI: 10.1021/acsmaterialslett.4c01833

Adélaïde Clavelin, Dat Le Thanh, Ivan Bobrikov, Marcus Fehse, Nicholas E Drewett, Gabriel A López, Damien Saurel, Montserrat Galceran

{"title":"Dehydration Conditions and Ultrafast Rehydration of Prussian White: Phase Transition Dynamics and Implications for Sodium-Ion Batteries.","authors":"Adélaïde Clavelin, Dat Le Thanh, Ivan Bobrikov, Marcus Fehse, Nicholas E Drewett, Gabriel A López, Damien Saurel, Montserrat Galceran","doi":"10.1021/acsmaterialslett.4c01833","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01833","url":null,"abstract":"Prussian White (PW) is a strategic cathode material for sodium-ion batteries, offering a high theoretical capacity and voltage. However, the crystalline structure and the electrochemical performance of PW strongly depend on the hydration level, which is difficult to control, leading to discrepancies in the results and interpretations presented in the literature. This work aims to provide a deeper insight into the dehydration process of PW materials and a better understanding of the impact of their fast rehydration, upon exposure to moisture, on their characterization. For this purpose, a Na1.87Mn[Fe(CN)6]0.99·1.99H2O sample was synthesized by a coprecipitation method and subsequently dehydrated to remove water. After thorough characterization, our findings show that drying parameters, such as temperature and pressure, strongly influence the post-drying result. Moreover, the dehydrated samples rehydrate within minutes of exposure to air, which may explain some discrepancies observed in the literature and highlights the necessity to work under fully air-tight conditions.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"6 11","pages":"5208-5214"},"PeriodicalIF":9.6,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11539934/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142602235","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

High-Areal-Capacity All-Solid-State Lithium Batteries Enabled by Electronically Conductive Li-Deficient LiNiO2 Cathode 利用电子导电锂负极实现高实际容量全固态锂电池

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-24 DOI: 10.1021/acsenergylett.4c0145710.1021/acsenergylett.4c01457

Ying Jiang, Xiang Wu, Guozhong Lu, Hui Feng, Jiefan Liu, Jiaxing Lv, Fushan Geng, Ming Shen* and Bingwen Hu*,

{"title":"High-Areal-Capacity All-Solid-State Lithium Batteries Enabled by Electronically Conductive Li-Deficient LiNiO2 Cathode","authors":"Ying Jiang, Xiang Wu, Guozhong Lu, Hui Feng, Jiefan Liu, Jiaxing Lv, Fushan Geng, Ming Shen* and Bingwen Hu*, ","doi":"10.1021/acsenergylett.4c0145710.1021/acsenergylett.4c01457","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01457https://doi.org/10.1021/acsenergylett.4c01457","url":null,"abstract":"All-solid-state lithium batteries (ASSLBs) with Ni-rich cathodes are promising candidates for achieving high energy and improved safety. However, their electrochemical performance is limited by cathode loading, especially in the absence of conductive agents. Herein, we utilize electronically conductive Li-deficient LiNiO2 (LD-LNO) to construct high-areal-capacity ASSLBs under high cathode loading. This LD-LNO shows an inherent enhanced electronic conductivity and minimal surface impurities. Electrochemical analysis combined with solid-state nuclear magnetic resonance spectroscopy demonstrates the mitigation of the detrimental H3 phase transition and the side reactions at the LD-LNO/Li6PS5Cl interface. As a result, LD-LNO-based ASSLBs achieve competitive cyclability and rate capability without the need for cathode modifications. A high reversible areal capacity of 15.2 mAh cm–2 is attained at 35 °C under a 133.8 mg cm–2 LD-LNO mass loading. This work sheds light on electronically conductive cathodes, providing a perspective for addressing the high cathode loading issue in ASSLBs.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5529–5538 5529–5538"},"PeriodicalIF":19.3,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608747","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Overcoming the Open-Circuit Voltage Losses in Narrow Bandgap Perovskites for All-Perovskite Tandem Solar Cells. 克服窄带隙过氧化物的开路电压损耗，实现全过氧化物串联太阳能电池。

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2024-10-23 eCollection Date: 2024-11-04 DOI: 10.1021/acsmaterialslett.4c01699

Yekitwork Abebe Temitmie, Muhammad Irfan Haider, Daniele T Cuzzupè, Lucia V Mercaldo, Stefan Kraner, Paola Delli Veneri, Amare Benor, Azhar Fakharuddin, Lukas Schmidt-Mende

{"title":"Overcoming the Open-Circuit Voltage Losses in Narrow Bandgap Perovskites for All-Perovskite Tandem Solar Cells.","authors":"Yekitwork Abebe Temitmie, Muhammad Irfan Haider, Daniele T Cuzzupè, Lucia V Mercaldo, Stefan Kraner, Paola Delli Veneri, Amare Benor, Azhar Fakharuddin, Lukas Schmidt-Mende","doi":"10.1021/acsmaterialslett.4c01699","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c01699","url":null,"abstract":"Narrow-bandgap (NBG) perovskite solar cells based on tin-lead mixed perovskite absorbers suffer from significant open-circuit voltage (V OC) losses due primarily to a high defect density and charge carrier recombination at the device interfaces. In this study, the V OC losses in NBG perovskite single junction cells (E g = 1.21 eV) are addressed. The optimized NBG subcell is then used to fabricate highly efficient all-perovskite tandem solar cells (TSCs). The improvement in the V OC is achieved via the addition of a thin poly(triarylamine) interlayer between the poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate) (PEDOT:PSS)-based hole transport layer (HTL) and the NBG perovskite. The optimal bilayer HTL results in a champion power conversion efficiency (PCE) of 20.3%, compared to 17.8% of the PEDOT:PSS-based control device. The V OC improvement of the single-junction NBG cell is also successfully transferred to all-perovskite TSC, resulting in a high V OC of 2.00 V and a PCE of 25.1%.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"6 11","pages":"5190-5198"},"PeriodicalIF":9.6,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11539106/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142602240","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Steric Hindrance-Derived Li+ Solvation to Enhance Lithium-Mediated Nitrogen Reduction 立体阻碍作用产生的 Li+ 溶胶增强锂介导的氮还原作用

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-23 DOI: 10.1021/acsenergylett.4c0262610.1021/acsenergylett.4c02626

Yebin Han, Chaeeun Lim, Youngbi Kim, Hyerim Baek, Sangmin Jeon, Jeong Woo Han* and Kijung Yong*,

{"title":"Steric Hindrance-Derived Li+ Solvation to Enhance Lithium-Mediated Nitrogen Reduction","authors":"Yebin Han, Chaeeun Lim, Youngbi Kim, Hyerim Baek, Sangmin Jeon, Jeong Woo Han* and Kijung Yong*, ","doi":"10.1021/acsenergylett.4c0262610.1021/acsenergylett.4c02626","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02626https://doi.org/10.1021/acsenergylett.4c02626","url":null,"abstract":"This study proposes a steric hindrance-derived electrolyte (STE) to generate Li+ anion-rich solvation structures to enhance the Li-mediated nitrogen reduction reaction (Li-NRR), a promising electrochemical green ammonia synthesis method. The STE applied methylation of the alpha proton in the tetrahydrofuran (THF) solvent, which dissolved lithium salts, leading to the weak solvation of Li+ and generating an anion-rich-solvated structure. The resultant anion-derived solid electrolyte interphase with thin and uniform inorganic properties improved the selectivity, energy efficiency (EE), and stability of the Li-NRR process. Additionally, the anion-rich solvation exhibited antireduction stability and inhibited electrolyte decomposition. Consequently, the STE achieved a 2-fold increase in Faradaic efficiency and NH3 yield rate (65.8% and 90.8 nmol cm–2 s–1, respectively) compared to the THF-single electrolyte (35.7% and 49.3 nmol cm–2 s–1) while increasing the EE by 1.5 times.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5509–5519 5509–5519"},"PeriodicalIF":19.3,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenergylett.4c02626","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608600","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enhancing Recoverable Bendability in High-Performance Ag2Se-Based Thermoelectrics through Plastic Processing 通过塑料加工增强 Ag2Se 基高性能热电半导体的可回收弯曲性

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-22 DOI: 10.1021/acsenergylett.4c0232710.1021/acsenergylett.4c02327

Wenjun Ding, Xinyi Shen, Ziyan Li, Zimin Fan, Zhiwei Chen, Juan Chen, Jun Luo*, Wen Li* and Yanzhong Pei*,

{"title":"Enhancing Recoverable Bendability in High-Performance Ag2Se-Based Thermoelectrics through Plastic Processing","authors":"Wenjun Ding, Xinyi Shen, Ziyan Li, Zimin Fan, Zhiwei Chen, Juan Chen, Jun Luo*, Wen Li* and Yanzhong Pei*, ","doi":"10.1021/acsenergylett.4c0232710.1021/acsenergylett.4c02327","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02327https://doi.org/10.1021/acsenergylett.4c02327","url":null,"abstract":"Urgent demand for a sustainable power supply for wearables promotes great efforts on the development of flexible thermoelectric devices. The elastic bendability allows the reservation of initial power and flexibility in inorganic thermoelectric films. The elasticity is related to the thickness engineeringly and the elastic strain scientifically, therefore guiding this work to focus on developing elastic thermoelectric generators using high-performing orthorhombic Ag2Se1–xSx films that thinned the bulks through multipass hot-rolling at ∼393 K. Such a plastic deformation enables a creation of dense dislocations and a refinement of grain and, thereby, a dramatic increase in the elastic strain, impressively securing a full recoverability in transport properties for the obtained films even after 100,000 times bending within a radius down to ∼3 mm. The resultant achievement of extraordinary specific power density of ∼5 μW/cm-K2 in a six-leg flexible device robustly demonstrates these alloys as a potentially sustainable power source for wearable electronics.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5483–5491 5483–5491"},"PeriodicalIF":19.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608136","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Regulating Reconstruction Activity of Cobalt Electrode for Optimized Water Oxidation 调节钴电极的重构活性，优化水氧化过程

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-22 DOI: 10.1021/acsenergylett.4c0234410.1021/acsenergylett.4c02344

Miao Wang, Ziyi Wang, Yunze Zhang, Yan Shi, Ting-Shan Chan, Shu-Chih Haw, Jian Wang, Hongsheng Wang, Siyuan Wang, Hao Fei, Ruoqi Liu, Tong Liu, Chang-Feng Yan and Jian Wang*,

{"title":"Regulating Reconstruction Activity of Cobalt Electrode for Optimized Water Oxidation","authors":"Miao Wang, Ziyi Wang, Yunze Zhang, Yan Shi, Ting-Shan Chan, Shu-Chih Haw, Jian Wang, Hongsheng Wang, Siyuan Wang, Hao Fei, Ruoqi Liu, Tong Liu, Chang-Feng Yan and Jian Wang*, ","doi":"10.1021/acsenergylett.4c0234410.1021/acsenergylett.4c02344","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02344https://doi.org/10.1021/acsenergylett.4c02344","url":null,"abstract":"Elucidating and regulating dynamic catalyst reconstruction are crucial for various electrocatalytic reactions. Here, we applied model fittings with operando characterizations to quantify the reconstruction activity (i.e., ability to reconstruct) of layered Co(OH)2 toward the oxygen evolution reaction (OER). By modulating the intercalation species into Co(OH)2, we governed distinct reconstruction thermodynamics and kinetics, with diverse mass changes and heterogeneous Co oxidation during the OER. We further established a volcano-type relationship between reconstruction activity and OER activity and identified that a moderate reconstruction activity, achieved by dual-anion intercalation, favored a high OER activity. This might result from its proper basal spacing that regulated the coupled ion (de)intercalation–electron transfer for reconstruction, leading to optimal Co for binding OER intermediates. The optimally reconstructed Co(OH)1.26Cl0.08(CO3)0.33·0.84 H2O delivered 1 A cm–2 at 1.78 V for anion-exchange membrane water electrolysis. This work laid the foundation for modulating reconstruction activities to benefit electrocatalysis.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5502–5508 5502–5508"},"PeriodicalIF":19.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608134","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Unveiling the Local Structure and the Ligand Field of Organic Cation Preintercalated Vanadate Cathode for Aqueous Zinc-Ion Batteries 揭示锌离子水电池有机阳离子预烧结钒酸盐阴极的局部结构和配体场

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-22 DOI: 10.1021/acsenergylett.4c0270910.1021/acsenergylett.4c02709

Heng Liu, Huanhuan Niu, Wei-Hsiang Huang, Ting Shen, Changyuan Li, Chun-Chi Chang, Menghao Yang, Chenlong Gao, Long Yang, Quan Zong, Yanzhong Pei, Guozhong Cao* and Chaofeng Liu*,

{"title":"Unveiling the Local Structure and the Ligand Field of Organic Cation Preintercalated Vanadate Cathode for Aqueous Zinc-Ion Batteries","authors":"Heng Liu, Huanhuan Niu, Wei-Hsiang Huang, Ting Shen, Changyuan Li, Chun-Chi Chang, Menghao Yang, Chenlong Gao, Long Yang, Quan Zong, Yanzhong Pei, Guozhong Cao* and Chaofeng Liu*, ","doi":"10.1021/acsenergylett.4c0270910.1021/acsenergylett.4c02709","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02709https://doi.org/10.1021/acsenergylett.4c02709","url":null,"abstract":"Layered vanadium-based materials have been extensively studied as promising cathode materials for aqueous zinc-ion batteries (AZIBs). However, challenges remain to achieve the desired high energy conversion efficiency and energy densities as well as long cycling stability requiring an in-depth understanding of the local and the electronic structure of a vanadium-based cathode, especially concerning the impacts on electrochemical potential and mass transfer in the electrochemical process. In this work, 1-butyl-1-methylpyrrolidinium cations are preintercalated into the layered hydrate vanadium pentoxide (V2O5·nH2O) and partially replace the electroneutral structural water, changing the local atomic environment. X-ray absorption spectroscopies demonstrate the V–O bond elongation and the distortion in the [VO6] octahedra, which alter the ligand field and brings the V 3d state to a lower energy level, ultimately leading to an increase in the electrochemical potential. It is also revealed that the preintercalated organic cations exert electrostatic interaction with lattice oxygen, stabilizing the layered structure and buffering lattice strain during cycling. Consequently, the modified cathode achieves a superior specific capacity of 412 mAh/g at 0.5 A/g and a capacity retention of 97% after 3000 cycles at 8 A/g. The unveiled correlation between local structure and electrochemical performance paves the way for optimizing the cathode materials by manipulating the local coordination environment.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5492–5501 5492–5501"},"PeriodicalIF":19.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608133","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Li2FeCl4 as a Cost-Effective and Durable Cathode for Solid-State Li-Ion Batteries 将 Li2FeCl4 用作固态锂离子电池具有成本效益且经久耐用的阴极

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-21 DOI: 10.1021/acsenergylett.4c0237610.1021/acsenergylett.4c02376

Zhantao Liu, Guangxing Zhang, Jakub Pepas, Yifan Ma and Hailong Chen*,

引用次数: 0

Sustainable Molecular Passivation via Heat-Induced Disaggregation and Redox Reactions for Inverted Perovskite Solar Cells 通过热诱导的解离和氧化还原反应实现可持续的分子钝化，用于反相包晶石太阳能电池

IF 19.3 1区化学

ACS Materials Letters Pub Date : 2024-10-21 DOI: 10.1021/acsenergylett.4c0222010.1021/acsenergylett.4c02220

Ziyi Li, Anxin Sun, Congcong Tian, Rongshan Zhuang, Yiting Zheng, Xiling Wu, Beilin Ouyang, Jiajun Du, Jingyu Cai, Jinling Chen, Teng Xue, Ran Li, Tiantian Cen, Yuyang Zhao, Kaibo Zhao, Qianwen Chen and Chun-Chao Chen*,

{"title":"Sustainable Molecular Passivation via Heat-Induced Disaggregation and Redox Reactions for Inverted Perovskite Solar Cells","authors":"Ziyi Li, Anxin Sun, Congcong Tian, Rongshan Zhuang, Yiting Zheng, Xiling Wu, Beilin Ouyang, Jiajun Du, Jingyu Cai, Jinling Chen, Teng Xue, Ran Li, Tiantian Cen, Yuyang Zhao, Kaibo Zhao, Qianwen Chen and Chun-Chao Chen*, ","doi":"10.1021/acsenergylett.4c0222010.1021/acsenergylett.4c02220","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02220https://doi.org/10.1021/acsenergylett.4c02220","url":null,"abstract":"Molecular materials with high structure-design freedom are used as new interface passivators to reduce nonradiative recombination in inverted perovskite solar cells (PSCs). However, most molecular modifiers are unable to achieve a long-term passivation effect due to self-aggregation. Here, the molecular modifier 1-methyl-2-thiomethyl-1H-imidazole-5-carboxylate (SMC) with ester and thiol groups is carefully developed. The ester groups weaken self-aggregation triggered by intermolecular hydrogen bonds, making such aggregations easier to disassemble during heating to form a net-like insulating layer with random openings, which dramatically increase charge transport. More importantly, the electron transfer between thiol and disulfide can accelerate the elimination of Pb0 and I2 by redox reactions to prevent phase separation. Ultimately, the optimized inverted PSCs with bandgaps of 1.68 and 1.55 eV showed surprising fill factors of 84.83% and 86.18%, resulting in champion efficiencies of 23.45% (certified 22.98%, which is the highest to date for wide-bandgap) and 25.71% (certified 25.28%), respectively. Remarkably, both unencapsulated devices maintained over 94% of their initial efficiency under maximum power point tracking for 600 h (50 °C) and 1000 h (65 °C), respectively, confirming impressive long-term operational stability.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"9 11","pages":"5471–5482 5471–5482"},"PeriodicalIF":19.3,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609052","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0