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Tuning Dimensions of CsPbBr3 Nanocrystals through Pb(II) Counter Anions: A Dance of Dimensions and Product Selectivity in Visible-Light Photocatalysis
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-04 DOI: 10.1021/acsenergylett.5c00033
Anupam Manna, Pravat Nayek, Prasenjit Mal
{"title":"Tuning Dimensions of CsPbBr3 Nanocrystals through Pb(II) Counter Anions: A Dance of Dimensions and Product Selectivity in Visible-Light Photocatalysis","authors":"Anupam Manna, Pravat Nayek, Prasenjit Mal","doi":"10.1021/acsenergylett.5c00033","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00033","url":null,"abstract":"The size tuning of perovskite nanocrystals has been extensively studied and is commonly influenced by factors such as reaction temperature, duration, ligand type, ligand chain length, and choice of halogen source. This study presents a cost-efficient strategy for precise control over the dimensions, shape, size, and phase, of nanocrystals by modulating Pb(II) counteranions during hot-injection synthesis. By employing diethyl 2-bromomalonate as the bromide precursor, distinct nanocrystal morphologies were achieved using different lead sources: lead acetate, lead bromide, lead oxide, and lead nitrate yielded 1D nanorods, 2D nanoplatelets, 3D nanocubes, and quantum dots (QDs), respectively. The resulting CsPbBr<sub>3</sub> nanocrystals exhibited high photoluminescence quantum yields (PLQY &gt; 90%) and prolonged excited-state lifetimes (τ ≈ 6.1–15.1 ns). Furthermore, these nanocrystals displayed variable photocatalytic efficiencies in radical cascade cyclization reactions involving <i>N</i>-alkyl/aryl-maleimide and <i>N</i>-phenyl glycine under visible light (blue LED) in dichloroethane. Notably, the reaction yields were strongly influenced by the distinct sizes and morphologies of the nanocrystals.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"1 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546824","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synergistic Bulk and Interface Engineering of Layered Oxide Cathodes for Na-Ion Batteries
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-04 DOI: 10.1021/acsenergylett.4c03601
Xu Yang, Yingfei Li, Xinyu Li, Ting Lin, Weiguang Lin, Peihua Li, Dongdong Xiao, Shurong Wang, Huilin Pan
{"title":"Synergistic Bulk and Interface Engineering of Layered Oxide Cathodes for Na-Ion Batteries","authors":"Xu Yang, Yingfei Li, Xinyu Li, Ting Lin, Weiguang Lin, Peihua Li, Dongdong Xiao, Shurong Wang, Huilin Pan","doi":"10.1021/acsenergylett.4c03601","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03601","url":null,"abstract":"Na-ion batteries (NIBs) hold promise for large-scale energy storage due to the abundance and low cost of Na resources, but their practical applications are still limited by the energy density and cycling stability of the cathodes. This study develops a synergistic bulk and interfacial modification strategy for O3-type NaNi<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> (NFM) cathode using CaHPO<sub>4</sub> (CP), integrating Ca doping and uniform NaPO<sub>3</sub> coating to enhance structural stability and interfacial robustness. The modified cathode (2%CP@NFM) delivers excellent performance, retaining 92% capacity over 300 cycles at 2 C, no capacity decay after 400 cycles at 5 C, and 83% capacity retention over 1000 cycles at 1 C in full-cells. Structural analyses reveal remarkable suppression of irreversible phase transitions, gas evolution, and transition metal ion dissolution issues of layered oxide cathodes. These findings highlight the potential of a low-cost CP modification strategy in achieving high-performance NIBs for sustainable energy storage.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"32 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539151","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synergistic Bulk and Interface Engineering of Layered Oxide Cathodes for Na-Ion Batteries
IF 19.3 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-04 DOI: 10.1021/acsenergylett.4c0360110.1021/acsenergylett.4c03601
Xu Yang, Yingfei Li, Xinyu Li, Ting Lin, Weiguang Lin, Peihua Li, Dongdong Xiao*, Shurong Wang and Huilin Pan*, 
{"title":"Synergistic Bulk and Interface Engineering of Layered Oxide Cathodes for Na-Ion Batteries","authors":"Xu Yang,&nbsp;Yingfei Li,&nbsp;Xinyu Li,&nbsp;Ting Lin,&nbsp;Weiguang Lin,&nbsp;Peihua Li,&nbsp;Dongdong Xiao*,&nbsp;Shurong Wang and Huilin Pan*,&nbsp;","doi":"10.1021/acsenergylett.4c0360110.1021/acsenergylett.4c03601","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03601https://doi.org/10.1021/acsenergylett.4c03601","url":null,"abstract":"<p >Na-ion batteries (NIBs) hold promise for large-scale energy storage due to the abundance and low cost of Na resources, but their practical applications are still limited by the energy density and cycling stability of the cathodes. This study develops a synergistic bulk and interfacial modification strategy for O3-type NaNi<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> (NFM) cathode using CaHPO<sub>4</sub> (CP), integrating Ca doping and uniform NaPO<sub>3</sub> coating to enhance structural stability and interfacial robustness. The modified cathode (2%CP@NFM) delivers excellent performance, retaining 92% capacity over 300 cycles at 2 C, no capacity decay after 400 cycles at 5 C, and 83% capacity retention over 1000 cycles at 1 C in full-cells. Structural analyses reveal remarkable suppression of irreversible phase transitions, gas evolution, and transition metal ion dissolution issues of layered oxide cathodes. These findings highlight the potential of a low-cost CP modification strategy in achieving high-performance NIBs for sustainable energy storage.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 3","pages":"1491–1498 1491–1498"},"PeriodicalIF":19.3,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143609026","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Nickel–Antimony Electrocatalyst for Durable Acidic Hydrogen Evolution Reaction in Proton Exchange Membrane Electrolyzers
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-03 DOI: 10.1021/acsenergylett.5c00233
Cheng Cai, Husileng Lee, Weili Shi, Yonghua Liu, Biaobiao Zhang, Licheng Sun, Tao Wang
{"title":"Nickel–Antimony Electrocatalyst for Durable Acidic Hydrogen Evolution Reaction in Proton Exchange Membrane Electrolyzers","authors":"Cheng Cai, Husileng Lee, Weili Shi, Yonghua Liu, Biaobiao Zhang, Licheng Sun, Tao Wang","doi":"10.1021/acsenergylett.5c00233","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00233","url":null,"abstract":"Developing a nonprecious alternative to platinum as hydrogen evolution reaction (HER) catalyst in a proton exchange membrane water electrolyzer (PEM-WE) has been a long-standing pursuit in electrochemical water splitting. Here, we report the theory-aided discovery of a noble-metal-free NiSb electrocatalyst with high stability and activity for acidic HER, continuously operating over 3000 h at 2 A cm<sup>–2</sup> and 60 °C with a cell voltage of 2.28 V in the PEM-WE. This NiSb catalyst was identified through a comprehensive stability and activity evaluation framework with computations, incorporating rigorous aqueous stability assessment via Pourbaix diagram analysis. Further experimental studies confirmed the successful synthesis of NiSb and impressive performance for acidic HER, verifying the computational predictions. The record-high durability, high activity, and low cost make NiSb a promising alternative to Pt for practical application in PEM-WE.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"29 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143532398","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Nickel–Antimony Electrocatalyst for Durable Acidic Hydrogen Evolution Reaction in Proton Exchange Membrane Electrolyzers
IF 19.3 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-03 DOI: 10.1021/acsenergylett.5c0023310.1021/acsenergylett.5c00233
Cheng Cai, Husileng Lee, Weili Shi, Yonghua Liu, Biaobiao Zhang*, Licheng Sun and Tao Wang*, 
{"title":"Nickel–Antimony Electrocatalyst for Durable Acidic Hydrogen Evolution Reaction in Proton Exchange Membrane Electrolyzers","authors":"Cheng Cai,&nbsp;Husileng Lee,&nbsp;Weili Shi,&nbsp;Yonghua Liu,&nbsp;Biaobiao Zhang*,&nbsp;Licheng Sun and Tao Wang*,&nbsp;","doi":"10.1021/acsenergylett.5c0023310.1021/acsenergylett.5c00233","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00233https://doi.org/10.1021/acsenergylett.5c00233","url":null,"abstract":"<p >Developing a nonprecious alternative to platinum as hydrogen evolution reaction (HER) catalyst in a proton exchange membrane water electrolyzer (PEM-WE) has been a long-standing pursuit in electrochemical water splitting. Here, we report the theory-aided discovery of a noble-metal-free NiSb electrocatalyst with high stability and activity for acidic HER, continuously operating over 3000 h at 2 A cm<sup>–2</sup> and 60 °C with a cell voltage of 2.28 V in the PEM-WE. This NiSb catalyst was identified through a comprehensive stability and activity evaluation framework with computations, incorporating rigorous aqueous stability assessment via Pourbaix diagram analysis. Further experimental studies confirmed the successful synthesis of NiSb and impressive performance for acidic HER, verifying the computational predictions. The record-high durability, high activity, and low cost make NiSb a promising alternative to Pt for practical application in PEM-WE.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 3","pages":"1483–1490 1483–1490"},"PeriodicalIF":19.3,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608861","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Shortcut for Commercialization of Perovskites Solar Cells by a Recycling and Remanufacturing Strategy
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-02 DOI: 10.1021/acsenergylett.5c00140
Zhaoboxun Bao, Yaotao Luo, Lina Wang, Jing Dou, Lihua Wang, Yue Ma, Yujiang Du, Yisha Lan, Cheng Zhu, Haining Chen, Huanping Zhou, Yang Bai, Qi Chen
{"title":"A Shortcut for Commercialization of Perovskites Solar Cells by a Recycling and Remanufacturing Strategy","authors":"Zhaoboxun Bao, Yaotao Luo, Lina Wang, Jing Dou, Lihua Wang, Yue Ma, Yujiang Du, Yisha Lan, Cheng Zhu, Haining Chen, Huanping Zhou, Yang Bai, Qi Chen","doi":"10.1021/acsenergylett.5c00140","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00140","url":null,"abstract":"Perovskite photovoltaics exhibit impressive power conversion efficiency (PCE) and cost-effective manufacturing, developing as the most promising photovoltaic technology for commercialization beyond silicon. However, stability and end-of-life hazards remain significant challenges. Module recycling and remanufacturing could reduce costs and minimize Lead contamination risk. This study proposes a Recycling and Remanufacturing (R&amp;R) strategy for perovskite-based PV technologies and evaluates their commercial viability by calculating the levelized cost of energy (LCOE). Our findings indicate that when the PCE and lifetime of PSC modules reach 20% and 7 years (31% and 8 years for 2-terminal; 30% and 8 years for 4-terminal perovskite-silicon tandems), respectively, it can achieve an LCOE of 7.75 Cents/kWh, making it commercially competitive with silicon technology. The R&amp;R strategy also minimizes the utilization of hazardous Pb, easing postprocessing pollution. These findings highlight the R&amp;R strategy as a viable end-of-life solution for perovskite technology, which could accelerate its commercialization.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"52 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143528202","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Shortcut for Commercialization of Perovskites Solar Cells by a Recycling and Remanufacturing Strategy
IF 19.3 1区 材料科学
ACS Energy Letters Pub Date : 2025-03-02 DOI: 10.1021/acsenergylett.5c0014010.1021/acsenergylett.5c00140
Zhaoboxun Bao, Yaotao Luo, Lina Wang, Jing Dou, Lihua Wang, Yue Ma, Yujiang Du, Yisha Lan, Cheng Zhu, Haining Chen, Huanping Zhou, Yang Bai* and Qi Chen, 
{"title":"A Shortcut for Commercialization of Perovskites Solar Cells by a Recycling and Remanufacturing Strategy","authors":"Zhaoboxun Bao,&nbsp;Yaotao Luo,&nbsp;Lina Wang,&nbsp;Jing Dou,&nbsp;Lihua Wang,&nbsp;Yue Ma,&nbsp;Yujiang Du,&nbsp;Yisha Lan,&nbsp;Cheng Zhu,&nbsp;Haining Chen,&nbsp;Huanping Zhou,&nbsp;Yang Bai* and Qi Chen,&nbsp;","doi":"10.1021/acsenergylett.5c0014010.1021/acsenergylett.5c00140","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00140https://doi.org/10.1021/acsenergylett.5c00140","url":null,"abstract":"<p >Perovskite photovoltaics exhibit impressive power conversion efficiency (PCE) and cost-effective manufacturing, developing as the most promising photovoltaic technology for commercialization beyond silicon. However, stability and end-of-life hazards remain significant challenges. Module recycling and remanufacturing could reduce costs and minimize Lead contamination risk. This study proposes a Recycling and Remanufacturing (R&amp;R) strategy for perovskite-based PV technologies and evaluates their commercial viability by calculating the levelized cost of energy (LCOE). Our findings indicate that when the PCE and lifetime of PSC modules reach 20% and 7 years (31% and 8 years for 2-terminal; 30% and 8 years for 4-terminal perovskite-silicon tandems), respectively, it can achieve an LCOE of 7.75 Cents/kWh, making it commercially competitive with silicon technology. The R&amp;R strategy also minimizes the utilization of hazardous Pb, easing postprocessing pollution. These findings highlight the R&amp;R strategy as a viable end-of-life solution for perovskite technology, which could accelerate its commercialization.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 3","pages":"1474–1482 1474–1482"},"PeriodicalIF":19.3,"publicationDate":"2025-03-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143609056","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Self-Passivation at the SnO2/Perovskite Interface
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-28 DOI: 10.1021/acsenergylett.5c00521
Kai-Ping Wang, Xue Dong, Ji-Zhe Yuan, Bo Wen, Jun He, Chuan-Jia Tong, Oleg V. Prezhdo
{"title":"Self-Passivation at the SnO2/Perovskite Interface","authors":"Kai-Ping Wang, Xue Dong, Ji-Zhe Yuan, Bo Wen, Jun He, Chuan-Jia Tong, Oleg V. Prezhdo","doi":"10.1021/acsenergylett.5c00521","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00521","url":null,"abstract":"Interfaces are crucial to the performance of solar cells, as they significantly affect charge transport. Using density functional theory and nonadiabatic molecular dynamics simulations, we reveal a self-passivation mechanism at the SnO<sub>2</sub>/CH<sub>3</sub>NH<sub>3</sub>PbI<sub>3</sub> interface to enhance the stability and efficiency of the device, which is mainly attributed to a benign iodine vacancy (V<sub>Iact</sub>). Unlike the typical defects of accelerating the charge recombination and reducing efficiency, this distinctive V<sub>Iact</sub> facilitates charge transfer and decelerates nonradiative recombination by passivating the potential trap states. Additionally, the benign V<sub>Iact</sub> at the interface reduces structural distortion and suppresses electron–vibration interactions, which in turn, extends the charge carrier lifetime and enhances the electron injection. Furthermore, V<sub>Iact</sub> exhibits both thermodynamic and kinetics stability. Our findings rationalize the high performance of SnO<sub>2</sub>-based perovskite solar cells and highlight the importance of the defect self-passivation strategy in optimizing interfacial properties for enhanced solar cell efficiency.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"66 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143526451","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Molecular Si-Cyclization Enables Versatile Organic Semiconductors for Durable Perovskite Solar Cells with 24.8% Efficiency
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-28 DOI: 10.1021/acsenergylett.5c00197
Zongyuan Yang, Zhaolong Ma, Zhe Wang, Mengyuan Li, Zhihui Wang, Hui Cheng, Xueping Zong, Suhao Yan, Mao Liang
{"title":"Molecular Si-Cyclization Enables Versatile Organic Semiconductors for Durable Perovskite Solar Cells with 24.8% Efficiency","authors":"Zongyuan Yang, Zhaolong Ma, Zhe Wang, Mengyuan Li, Zhihui Wang, Hui Cheng, Xueping Zong, Suhao Yan, Mao Liang","doi":"10.1021/acsenergylett.5c00197","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00197","url":null,"abstract":"Employing large fused-aromatic heterocycles to facilitate hole extraction and transport has been shown to significantly enhance the photovoltaic performance of perovskite solar cells (PSCs), but this approach typically results in a low intrinsic solubility and reduced device durability. In this study, we have developed two tetrathienosilole (TTS)-cored hole transporting materials (HTMs) through molecular <i>Si</i>-cyclization, aiming to address this common trade-off effect. The optimized atomic arrangement and enhanced planarity impart the resultant TTS-based HTMs with stronger interfacial interactions with the perovskite. Meanwhile, the perpendicular orientation of side-chains induced by the sp<sup>3</sup>-hybridized Si atom effectively improves the film morphology. By incorporating additional thiophene π-bridges, the <i>Si</i>-cyclized <b>WH12</b> exhibits a high hole mobility and film-formation quality. Consequently, the corresponding FAPbI<sub>3</sub>-based PSCs achieved a record efficiency of 24.8% with exceptional operational durability (<i>T</i><sub>80</sub> &gt; 1000 h). This work highlights the significant potential and versatility of the <i>Si</i>-cyclization strategy, opening new avenues for designing multifunctional molecular semiconductors.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"15 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518560","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Molecular Si-Cyclization Enables Versatile Organic Semiconductors for Durable Perovskite Solar Cells with 24.8% Efficiency
IF 19.3 1区 材料科学
ACS Energy Letters Pub Date : 2025-02-28 DOI: 10.1021/acsenergylett.5c0019710.1021/acsenergylett.5c00197
Zongyuan Yang, Zhaolong Ma, Zhe Wang, Mengyuan Li, Zhihui Wang*, Hui Cheng, Xueping Zong*, Suhao Yan* and Mao Liang*, 
{"title":"Molecular Si-Cyclization Enables Versatile Organic Semiconductors for Durable Perovskite Solar Cells with 24.8% Efficiency","authors":"Zongyuan Yang,&nbsp;Zhaolong Ma,&nbsp;Zhe Wang,&nbsp;Mengyuan Li,&nbsp;Zhihui Wang*,&nbsp;Hui Cheng,&nbsp;Xueping Zong*,&nbsp;Suhao Yan* and Mao Liang*,&nbsp;","doi":"10.1021/acsenergylett.5c0019710.1021/acsenergylett.5c00197","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00197https://doi.org/10.1021/acsenergylett.5c00197","url":null,"abstract":"<p >Employing large fused-aromatic heterocycles to facilitate hole extraction and transport has been shown to significantly enhance the photovoltaic performance of perovskite solar cells (PSCs), but this approach typically results in a low intrinsic solubility and reduced device durability. In this study, we have developed two tetrathienosilole (TTS)-cored hole transporting materials (HTMs) through molecular <i>Si</i>-cyclization, aiming to address this common trade-off effect. The optimized atomic arrangement and enhanced planarity impart the resultant TTS-based HTMs with stronger interfacial interactions with the perovskite. Meanwhile, the perpendicular orientation of side-chains induced by the sp<sup>3</sup>-hybridized Si atom effectively improves the film morphology. By incorporating additional thiophene π-bridges, the <i>Si</i>-cyclized <b>WH12</b> exhibits a high hole mobility and film-formation quality. Consequently, the corresponding FAPbI<sub>3</sub>-based PSCs achieved a record efficiency of 24.8% with exceptional operational durability (<i>T</i><sub>80</sub> &gt; 1000 h). This work highlights the significant potential and versatility of the <i>Si</i>-cyclization strategy, opening new avenues for designing multifunctional molecular semiconductors.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 3","pages":"1448–1456 1448–1456"},"PeriodicalIF":19.3,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608778","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","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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