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Magnetism-Functionalized Lanthanide MOF-on-MOF with Plasmonic Differential Signal Amplification for Ultrasensitive Fluorescence Immunoassays. 磁性功能化镧系元素 MOF-on-MOF,用于超灵敏荧光免疫测定的等离子体差分信号放大。
IF 8.2 1区 化学
ACS Sensors Pub Date : 2024-11-18 DOI: 10.1021/acssensors.4c02505
Tianxiang Hang, Ciyang Zhang, Fubin Pei, Ming Yang, Fengyun Wang, Mingzhu Xia, Qingli Hao, Wu Lei
{"title":"Magnetism-Functionalized Lanthanide MOF-on-MOF with Plasmonic Differential Signal Amplification for Ultrasensitive Fluorescence Immunoassays.","authors":"Tianxiang Hang, Ciyang Zhang, Fubin Pei, Ming Yang, Fengyun Wang, Mingzhu Xia, Qingli Hao, Wu Lei","doi":"10.1021/acssensors.4c02505","DOIUrl":"https://doi.org/10.1021/acssensors.4c02505","url":null,"abstract":"<p><p>The successful application of fluorescence immunoassays for clinical diagnosis requires stable photoluminescent materials and highly efficient signal amplification strategies. In this work, the magnetism-functionalized lanthanide MOF-on-MOF (Fe<sub>3</sub>O<sub>4</sub>@SiO<sub>2</sub>@MOF-on-MOF) was synthesized through intermolecular (van der Waals) interaction-assisted growth and further homogeneous epitaxial growth, which significantly improved the fluorescence performances and uncovered the underlying mechanism. The quantum chemical theory calculation and experimental studies revealed that the introduced magnetic Fe<sub>3</sub>O<sub>4</sub>@SiO<sub>2</sub> not only endowed magnetic separation capability but also promoted fluorescence performances, which increased the energy transfer of the intersystem crossing process and suppressed the luminescence of ligands and aggregation-induced quenching. Furthermore, the plasmonic Ag/Au nanocages were developed as highly efficient fluorescence quenchers to improve the sensitivity of the fluorescence immunoassay. On the basis of the proposed differential signal amplification (DSA) strategy, the immunoassay displayed superior detection ability, with a limit of detection of 0.13 pg·mL<sup>-1</sup> for severe acute respiratory syndrome coronavirus 2 nucleocapsid protein. The designed magnetic lanthanide MOF-on-MOF and proposed DSA strategy give new insights into ultrasensitive fluorescence immunoassays.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666405","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
The Cross-Sensitivity of Chemiresistive Gas Sensors: Nature, Methods, and Peculiarities: A Systematic Review. 化学电阻式气体传感器的交叉灵敏度:性质、方法和特殊性:系统综述。
IF 8.2 1区 化学
ACS Sensors Pub Date : 2024-11-18 DOI: 10.1021/acssensors.4c02097
Amanzhol Turlybekuly, Yernar Shynybekov, Baktiyar Soltabayev, Gani Yergaliuly, Almagul Mentbayeva
{"title":"The Cross-Sensitivity of Chemiresistive Gas Sensors: Nature, Methods, and Peculiarities: A Systematic Review.","authors":"Amanzhol Turlybekuly, Yernar Shynybekov, Baktiyar Soltabayev, Gani Yergaliuly, Almagul Mentbayeva","doi":"10.1021/acssensors.4c02097","DOIUrl":"https://doi.org/10.1021/acssensors.4c02097","url":null,"abstract":"<p><p>The evaluation of selectivity/cross-sensitivity is one of the most important tests for gas sensor development, particularly that based on chemiresistive technology. It is known that chemiresistive gas sensors suffer from low selectivity when they provide sensitivity to several analytes. Typically, selectivity testing involves independently assessing a sensor's response to a specific gas. However, there is a growing need to evaluate performance with interfering gases or gas mixtures since gas sensors are always exposed to gas mixtures in practice. Despite the great importance of selectivity characterization, currently, there are no standard methods of selectivity tests at conditions when target gas coexists with interfering gas compounds, which mimics real conditions. We outlined the four main methods researchers use to evaluate the cross-sensitivity of gas sensors. It highlights key aspects of selectivity test performance, assessment methodologies, and procedure features, attempting to classify them by their distinct characteristics. This review covers the essentials of gas properties, adsorption and desorption processes, and gas molecule interactions. Finally, we tried to address the lack of standardized protocols for evaluating chemiresistive gas sensors' cross-sensitivity to interfering gases and guide researchers.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646047","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
SABRE-SHEATH Hyperpolarization of [1,5-13C2]Z-OMPD for Noninvasive pH Sensing. SABRE-SHEATH 超极化[1,5-13C2]Z-OMPD,用于无创 pH 值传感。
IF 8.2 1区 化学
ACS Sensors Pub Date : 2024-11-18 DOI: 10.1021/acssensors.4c01102
Mustapha B Abdulmojeed, Martin Grashei, Seth Dilday, Pascal Wodtke, Stephen McBride, Atli Davidsson, Erica Curran, Keilian MacCulloch, Austin Browning, Patrick TomHon, Andreas B Schmidt, Eduard Y Chekmenev, Franz Schilling, Thomas Theis
{"title":"SABRE-SHEATH Hyperpolarization of [1,5-<sup>13</sup>C<sub>2</sub>]Z-OMPD for Noninvasive pH Sensing.","authors":"Mustapha B Abdulmojeed, Martin Grashei, Seth Dilday, Pascal Wodtke, Stephen McBride, Atli Davidsson, Erica Curran, Keilian MacCulloch, Austin Browning, Patrick TomHon, Andreas B Schmidt, Eduard Y Chekmenev, Franz Schilling, Thomas Theis","doi":"10.1021/acssensors.4c01102","DOIUrl":"10.1021/acssensors.4c01102","url":null,"abstract":"<p><p>Hyperpolarized (HP) <sup>13</sup>C-labeled probes are emerging as promising agents to noninvasively image pH in vivo. HP [1,5-<sup>13</sup>C<sub>2</sub>]Z-OMPD (Z-4-methyl-2-oxopent-3-enedioic acid) in particular has recently been used to simultaneously report on kidney perfusion, filtration, and pH homeostasis, in addition to the ability to detect local tumor acidification. In previous studies, dissolution dynamic nuclear polarization was used to hyperpolarize Z-OMPD. Here, we pioneered the hyperpolarization of [1,5-<sup>13</sup>C<sub>2</sub>]Z-OMPD via SABRE-SHEATH (signal amplification by reversible exchange in shield enabling alignment transfer to heteronuclei), which is relatively simple and fast and promises to be highly scalable. With SABRE-SHEATH, we achieve enhancement values of ∼3950 and ∼2400 at 1.1 T (<i>P</i><sub>13C</sub> = 0.4 and 0.25%) on the labeled C-1 and C-5 positions of Z-OMPD. Density functional theory calculations at the B3LYP level of theory were used to investigate possible binding modes of Z-OMPD on the iridium-based polarization transfer catalyst. The experimental and theoretical results suggest that the equatorial binding mode to the catalyst, where Z-OMPD binds to the catalyst at both C-1 and C-5 carboxylate positions, is the most stable complex. The HP signals were used to measure the Z-OMPD chemical shift as a function of pH showing an ∼3 ppm shift across pH 4-11. This work lays a foundation for the development of a simple, low-cost hyperpolarization technique to image pH.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646031","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
Surface Potential Homogenization Improves Perovskite Solar Cell Performance 表面电位均匀化提高了包晶体太阳能电池的性能
IF 27.8 1区 化学
ACS Sensors Pub Date : 2024-11-14 DOI: 10.1002/aenm.202404755
Yao Xu, Jiangkai Yu, Songtao Liu, Fei Tang, Nanxi Ma, Kai Zhang, Fei Huang
{"title":"Surface Potential Homogenization Improves Perovskite Solar Cell Performance","authors":"Yao Xu, Jiangkai Yu, Songtao Liu, Fei Tang, Nanxi Ma, Kai Zhang, Fei Huang","doi":"10.1002/aenm.202404755","DOIUrl":"https://doi.org/10.1002/aenm.202404755","url":null,"abstract":"The synthesis of multicomponent metal halide perovskites (MHPs) by cationic and/or halide alloying allows band gap tuning, optimizing performance and improving stability. However, these multicomponent materials often suffer from compositional, structural, and property inhomogeneities, leading to uneven carrier transport and significant non-radiative recombination losses in lead halide perovskites. While many researchers have focused on the aggregation of perovskite halide ions, the impact of the surface potential has received relatively less attention. In this study, the multifunctional ionic liquid 1-allyl-3-methylimidazole dicyanamide (AMI) is introduced into the perovskite precursor to effectively regulate the surface potential of the perovskite layer. This approach inhibits non-radiative recombination, enhances carrier injection, and improves device performance. Surface potential homogenization within the perovskite layer leads to simultaneous improvements in both the efficiency and stability of perovskite solar cells. For wide-bandgap perovskites (1.81 eV), the optimal power conversion efficiency (PCE) reaches 20.44%, with an open-circuit voltage (<i>V</i><sub>oc</sub>) of 1.339 V, a short-circuit current density (<i>J</i><sub>sc</sub>) of 17.92 mA cm<sup>−2</sup>, and a high fill factor (FF) of 85%. This strategy also proved effective for conventional bandgap perovskite solar cells (PSCs) (1.53 eV), leading to a significant increase in performance, with the PCE increasing from 23.22% to 25.41%.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"78 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610440","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
Ultrasensitive, Fast-Response, and Stretchable Temperature Microsensor Based on a Stable Encapsulated Organohydrogel Film for Wearable Applications. 基于可穿戴应用的稳定封装有机水凝胶薄膜的超灵敏、快速响应和可拉伸温度微传感器
IF 8.2 1区 化学
ACS Sensors Pub Date : 2024-11-14 DOI: 10.1021/acssensors.4c02677
Hao Wang, Dijie Yao, Yibing Luo, Bizhang Zhong, Yiqun Gu, Hongjing Wu, Bo-Ru Yang, Chunwei Li, Kai Tao, Jin Wu
{"title":"Ultrasensitive, Fast-Response, and Stretchable Temperature Microsensor Based on a Stable Encapsulated Organohydrogel Film for Wearable Applications.","authors":"Hao Wang, Dijie Yao, Yibing Luo, Bizhang Zhong, Yiqun Gu, Hongjing Wu, Bo-Ru Yang, Chunwei Li, Kai Tao, Jin Wu","doi":"10.1021/acssensors.4c02677","DOIUrl":"https://doi.org/10.1021/acssensors.4c02677","url":null,"abstract":"<p><p>Ionic conductive hydrogel-based temperature sensors have emerged as promising candidates due to their good stretchability and biocompatibility. However, the unsatisfactory sensitivity, sluggish response/recovery speed, and poor environmental stability limit their applications for accurate long-term health monitoring and robot perception, especially in extreme environments. To address these concerns, here, the stretchable temperature sensors based on a double-side elastomer-encapsulated thin-film organohydrogel (DETO) architecture are proposed with impressive performance. It is found that the water-polyol binary solvent, organohydrogel film, and sandwiched device structure play important roles in the temperature sensing performance. By modifying the composition of binary solvent and thicknesses of organohydrogel and elastomer films, the DETO microsensors realize a thickness of only 380 μm, unprecedented temperature sensitivity (37.96%/°C), fast response time (6.01 s) and recovery time (10.53 s), wide detection range (25-95.7 °C), and good stretchability (40% strain), which are superior to those of conventional hydrogel-based sensors. Furthermore, the device displays good environmental stability with negligible dehydration and prolonged operation duration. With these attributes, the wearable sensor is exploited for the real-time monitoring of various physiological signals such as human skin temperature and respiration patterns as well as temperature perception for robots.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142612570","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
Efficient and Stable Organic Solar Cells Achieved by Synergistic Optimization of Extended End-Capped Groups and Fluorinated Quinoxaline Central Cores in Nonfullerene Acceptors 通过协同优化非富勒烯受体中的扩展端帽基团和氟化喹喔啉中心核实现高效稳定的有机太阳能电池
IF 27.8 1区 化学
ACS Sensors Pub Date : 2024-11-14 DOI: 10.1002/aenm.202403806
Chi Zhang, Yanan Shi, Jing Tao, Jianqi Zhang, Hao Zhang, Dingding Qiu, Caixuan Wang, Chenyang Tian, Zhixiang Wei, Kun Lu
{"title":"Efficient and Stable Organic Solar Cells Achieved by Synergistic Optimization of Extended End-Capped Groups and Fluorinated Quinoxaline Central Cores in Nonfullerene Acceptors","authors":"Chi Zhang, Yanan Shi, Jing Tao, Jianqi Zhang, Hao Zhang, Dingding Qiu, Caixuan Wang, Chenyang Tian, Zhixiang Wei, Kun Lu","doi":"10.1002/aenm.202403806","DOIUrl":"https://doi.org/10.1002/aenm.202403806","url":null,"abstract":"Molecular stacking behavior exerts a significant influence on the blend film morphology of organic solar cells (OSCs), further affecting device performance and stability. Modulation of the molecular structure, such as central unit and end-group, can profoundly impact this process. Herein, four quinoxaline (Qx)-fused-core-based non-fullerene acceptors (NFAs), Qx-N4F and Qx-<i>o/m/p</i>-N4F are synthesized combining π-extended end-groups and optimized central units. The isomeric fluorinated central units lead to changes in the local dipole moments and electrostatic potential distribution, which influences the molecular stacking pattern and photoelectronic properties of NFAs. Consequently, binary and ternary devices based on PM6:Qx-<i>p</i>-N4F achieve superior power conversion efficiencies (PCE) of up to 18.75% and 19.48%, respectively. Grazing-incidence wide-angle X-ray scattering (GIWAXS) characterization reveals Qx-<i>p</i>-N4F's stronger crystallinity, aggregation, and donor–acceptor interactions, which can separately enhance short-circuit current density (<i>J</i><sub>SC</sub>) and fill factor (FF) through higher phase purity and tighter molecular stacking based on maintaining more donor–acceptor interfaces. Furthermore, PM6:Qx-<i>p</i>-N4F-based devices demonstrate exceptional thermal stability, retaining 93.2% of the initial PCE value after 3000 h of heating due to the best morphological stability with the most stable stacking structure. These results underscore the significance of synergistic optimization of NFAs through conjugation expansion and halogenation substitution for obtaining efficient and stable OSCs.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"11 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142610394","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
PbSe Thermoelectrics: Efficient Candidates for Power Generation and Cooling 硒化铅热电:用于发电和冷却的高效候选材料
IF 27.8 1区 化学
ACS Sensors Pub Date : 2024-11-13 DOI: 10.1002/aenm.202404251
Shibo Liu, Bingchao Qin, Li-Dong Zhao
{"title":"PbSe Thermoelectrics: Efficient Candidates for Power Generation and Cooling","authors":"Shibo Liu, Bingchao Qin, Li-Dong Zhao","doi":"10.1002/aenm.202404251","DOIUrl":"https://doi.org/10.1002/aenm.202404251","url":null,"abstract":"Thermoelectric materials enable efficient and clean conversion between heat and electricity, offering significant application prospects in waste heat recovery and solid-state cooling. Lead selenide (PbSe) is a more abundant and cost-effective alternative to PbTe with promising potential for mid-temperature applications. However, things have changed very recently with the discovery of the traditional power generator PbSe being rather competitive as a thermoelectric cooler, opening new avenues for investigating this compound. This review aims to comb how the research achievements and promising performance of PbSe have shifted from medium to near-room temperatures, by comprehensively discussing various strategies to enhance the thermoelectric efficiency at different temperature ranges. Subsequently, it is reviewed how these advances in materials have triggered deep investigations on constructing high-efficiency power generation and cooling devices based on PbSe. Finally, a personal summary and outlook are presented on how to fully exploit the high-ranged thermoelectric performance of PbSe materials and manufacture high-efficiency power generators and coolers, thus promoting practical applications in the future.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"5 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601970","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
Interfacial Engineering-Assisted Energy Level Modulation Enhances the Photoelectrochemical Water Oxidation Performance of Bismuth Vanadate Photoanodes 界面工程辅助能级调制增强了钒酸铋光阳极的光电化学水氧化性能
IF 27.8 1区 化学
ACS Sensors Pub Date : 2024-11-13 DOI: 10.1002/aenm.202404477
Kaige Tian, Zhuo Xu, Hua Yang, Guilin Chen, Pengfei An, Jing Zhang, Shengzhong (Frank) Liu, Junqing Yan
{"title":"Interfacial Engineering-Assisted Energy Level Modulation Enhances the Photoelectrochemical Water Oxidation Performance of Bismuth Vanadate Photoanodes","authors":"Kaige Tian, Zhuo Xu, Hua Yang, Guilin Chen, Pengfei An, Jing Zhang, Shengzhong (Frank) Liu, Junqing Yan","doi":"10.1002/aenm.202404477","DOIUrl":"https://doi.org/10.1002/aenm.202404477","url":null,"abstract":"BiVO<sub>4</sub> faces significant challenges for widespread application in photoelectrochemical (PEC) water oxidation due to its poor hole transport ability, high surface defect density, and sluggish water oxidation reaction kinetics. Employing interfacial engineering to assist in energy level modulation is an effective strategy to address these challenges. Herein, a CuCrO<sub>2</sub> hole transport layer (HTL) is coupled and further grew NiCo-MOF in situ to prepare a NiCo-MOF-CuCrO<sub>2</sub>-BiVO<sub>4</sub> composite photoanode. The novel composite photoanode not only achieves a photocurrent density of 5.75 mA cm<sup>−2</sup> at 1.23 V versus a reversible hydrogen electrode (vs RHE) but also maintains stable operation for over 24 h. Comprehensive physicochemical characterization and density-functional theory calculations confirm that the built-in electric field generated by the p–n heterojunction formed between the CuCrO<sub>2</sub> HTL and BiVO<sub>4</sub> photoanode enhances the hole transport ability. Moreover, the NiCo-MOF chelated on the photoanode surface not only passivates the surface defect states but also accelerates the kinetics of the water oxidation reaction. Under the synergistic effect of dual modification, the PEC water oxidation performance of the BiVO<sub>4</sub> photoanode is dramatically improved. This pioneering work presents a MOF/HTL/BiVO<sub>4</sub> configuration that provides a blueprint for the future development of integrated photoanodes for efficient solar energy conversion.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"20 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142602032","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
Impact of Ion Migration on the Performance and Stability of Perovskite-Based Tandem Solar Cells 离子迁移对基于包晶石的串联太阳能电池的性能和稳定性的影响
IF 27.8 1区 化学
ACS Sensors Pub Date : 2024-11-13 DOI: 10.1002/aenm.202400720
Sahil Shah, Fengjiu Yang, Eike Köhnen, Esma Ugur, Mark Khenkin, Jarla Thiesbrummel, Bor Li, Lucas Holte, Sebastian Berwig, Florian Scherler, Paria Forozi, Jonas Diekmann, Francisco Peña-Camargo, Marko Remec, Nikhil Kalasariya, Erkan Aydin, Felix Lang, Henry Snaith, Dieter Neher, Stefaan De Wolf, Carolin Ulbrich, Steve Albrecht, Martin Stolterfoht
{"title":"Impact of Ion Migration on the Performance and Stability of Perovskite-Based Tandem Solar Cells","authors":"Sahil Shah, Fengjiu Yang, Eike Köhnen, Esma Ugur, Mark Khenkin, Jarla Thiesbrummel, Bor Li, Lucas Holte, Sebastian Berwig, Florian Scherler, Paria Forozi, Jonas Diekmann, Francisco Peña-Camargo, Marko Remec, Nikhil Kalasariya, Erkan Aydin, Felix Lang, Henry Snaith, Dieter Neher, Stefaan De Wolf, Carolin Ulbrich, Steve Albrecht, Martin Stolterfoht","doi":"10.1002/aenm.202400720","DOIUrl":"https://doi.org/10.1002/aenm.202400720","url":null,"abstract":"The stability of perovskite-based tandem solar cells (TSCs) is the last major scientific/technical challenge to be overcome before commercialization. Understanding the impact of mobile ions on the TSC performance is key to minimizing degradation. Here, a comprehensive study that combines an experimental analysis of ionic losses in Si/perovskite and all-perovskite TSCs using scan-rate-dependent current–voltage (<i>J–V</i>) measurements with drift-diffusion simulations is presented. The findings demonstrate that mobile ions have a significant influence on the tandem cell performance lowering the ion-freeze power conversion efficiency from &gt;31% for Si/perovskite and &gt;30% for all-perovskite tandems to ≈28% in steady-state. Moreover, the ions cause a substantial hysteresis in Si/perovskite TSCs at high scan speeds (400 s<sup>−1</sup>), and significantly influence the performance degradation of both devices through internal field screening. Additionally, for all-perovskite tandems, subcell-dominated <i>J–V</i> characterization reveals more pronounced ionic losses in the wide-bandgap subcell during aging, which is attributed to its tendency for halide segregation. This work provides valuable insights into ionic losses in perovskite-based TSCs which helps to separate ion migration-related degradation modes from other degradation mechanisms and guides targeted interventions for enhanced subcell efficiency and stability.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"38 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601965","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
In–Li Counter Electrodes in Solid-State Batteries – A Comparative Approach on Kinetics, Microstructure, and Chemomechanics 固态电池中的铟-锂反电极--动力学、微观结构和化学机械学的比较方法
IF 27.8 1区 化学
ACS Sensors Pub Date : 2024-11-13 DOI: 10.1002/aenm.202404055
Christoph D. Alt, Sören Keuntje, Inga L. Schneider, Johannes Westphal, Philip Minnmann, Janis K. Eckhardt, Klaus Peppler, Jürgen Janek
{"title":"In–Li Counter Electrodes in Solid-State Batteries – A Comparative Approach on Kinetics, Microstructure, and Chemomechanics","authors":"Christoph D. Alt, Sören Keuntje, Inga L. Schneider, Johannes Westphal, Philip Minnmann, Janis K. Eckhardt, Klaus Peppler, Jürgen Janek","doi":"10.1002/aenm.202404055","DOIUrl":"https://doi.org/10.1002/aenm.202404055","url":null,"abstract":"A key challenge for solid-state batteries is the fabrication of high-capacity cathodes with high area loading and good rate performance. To reliably quantify the performance of high-capacity cathodes, electrochemically stable, and high-rate counter electrodes are essential. Otherwise, a three-electrode setup is required. In–Li alloy electrodes are used for years in a kind of standard approach, since these seem to offer stable operation. In this comparative study, seven preparation methods for In–Li electrodes are examined, determining their suitability for cathode testing. The microstructure of a planar (i.e., foil) and a particle-based (i.e., composite) anode configuration is analyzed in more detail. Their rate-dependent electrode performance as well as electrochemical and chemomechanical reversibility in full-cell configuration are analyzed. The combined results demonstrate the limitations of In–Li electrodes for high-capacity testing, especially at high rates, while confirming their suitability for simple lab-scale testing. Preparation significantly influences the electrode microstructure and kinetics, consequently impacting the performance benchmarks of cathodes. These findings underscore both the challenges involved in applying In–Li counter electrodes and the resulting limited comparability of results from different laboratories.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"36 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601981","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
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