ACS Energy Letters 最新文献_第5页

Tracking Local pH Dynamics during Water Electrolysis via In-Line Continuous Flow Raman Spectroscopy 通过在线连续流拉曼光谱跟踪水电解过程中的局部pH动态

IF 19.3 1区材料科学

ACS Energy Letters Pub Date : 2025-04-03 DOI: 10.1021/acsenergylett.5c0058210.1021/acsenergylett.5c00582

Raul A. Marquez, Jay T. Bender, Shashwati C. da Cunha, Ashton M. Aleman, Amaresh Sahu, Venkat Ganesan, Delia J. Milliron, Joaquin Resasco, Thomas F. Jaramillo and C. Buddie Mullins*,

{"title":"Tracking Local pH Dynamics during Water Electrolysis via In-Line Continuous Flow Raman Spectroscopy","authors":"Raul A. Marquez, Jay T. Bender, Shashwati C. da Cunha, Ashton M. Aleman, Amaresh Sahu, Venkat Ganesan, Delia J. Milliron, Joaquin Resasco, Thomas F. Jaramillo and C. Buddie Mullins*, ","doi":"10.1021/acsenergylett.5c0058210.1021/acsenergylett.5c00582","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00582https://doi.org/10.1021/acsenergylett.5c00582","url":null,"abstract":"The performance of electrochemical devices, which play a critical role in decarbonization efforts, is often governed by proton-coupled electron transfer reactions at the electrode–electrolyte interface. These reactions are highly sensitive to the complex and dynamic microenvironment present at the electrode surface. However, characterizing this environment─particularly monitoring interfacial pH and its evolution under reaction conditions─remains challenging, necessitating the development of advanced analytical tools. Here, we introduce in-line continuous flow Raman spectroscopy (CFRS) as a spectroelectrochemical platform for quantifying interfacial pH swings generated during water-splitting. By monitoring phosphate ion speciation and controlling the hydrodynamics with a flow cell, we measure pH swings as a function of current density, flow rate, and distance from the electrode. Comparison with theoretical models reveals the impact of bulk pH, boundary layer thickness, and bubble dynamics at high current densities. Collectively, these findings establish CFRS as a platform for quantitatively investigating pH dynamics, offering critical insights for advancing electrochemical energy conversion technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 4","pages":"2075–2083 2075–2083"},"PeriodicalIF":19.3,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143818909","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

Lead-Free Perovskite Tandem Solar Cells with Wide Bandgap Tin Perovskite and CIGS 具有宽禁带锡钙钛矿和CIGS的无铅钙钛矿串联太阳能电池

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-03 DOI: 10.1021/acsenergylett.5c00163

Hua̅n Bì, Zheng Zhang, Takeshi Kitamura, Gaurav Kapil, Ajay Kumar Baranwal, Mengmeng Chen, Liang Wang, Jiaqi Liu, Qing Shen, Shuzi Hayase

{"title":"Lead-Free Perovskite Tandem Solar Cells with Wide Bandgap Tin Perovskite and CIGS","authors":"Hua̅n Bì, Zheng Zhang, Takeshi Kitamura, Gaurav Kapil, Ajay Kumar Baranwal, Mengmeng Chen, Liang Wang, Jiaqi Liu, Qing Shen, Shuzi Hayase","doi":"10.1021/acsenergylett.5c00163","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00163","url":null,"abstract":"Wide-bandgap (WBG) tin perovskite solar cells offer a promising solution for the development of multijunction and nontoxic photovoltaic devices. However, rapid crystallization of the perovskite film always results in numerous defects within it, creating nonradiative recombination sites that impair both the efficiency and the stability of the devices. In this work, a ferrocene-based additive, 1,1-bis(diphenylphosphino)ferrocene-palladium(II) dichloride dichloromethane complex (Pd(dppf)Cl2), was introduced to enable the fabrication of high-quality perovskite films and high-efficiency perovskite devices. The functional groups in Pd(dppf)Cl2 (e.g., benzene rings, Cl, etc.) interact with the perovskite to enhance the perovskite film quality. Additionally, the reducibility of ferrocene offers an effective approach to improve film properties, as ferrocene can efficiently reduce Sn4+ to Sn2+ in both the solution and the film. Finally, the single junction device with a Pd(dppf)Cl2 additive achieved a power conversion efficiency (PCE) of 11.52% and demonstrated improved stability. Furthermore, a fully lead-free tandem device based on WBG Sn PSCs was fabricated, achieving a remarkable PCE of 14.51%.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"230 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776220","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

Tracking Local pH Dynamics during Water Electrolysis via In-Line Continuous Flow Raman Spectroscopy 通过在线连续流拉曼光谱跟踪水电解过程中的局部pH动态

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-03 DOI: 10.1021/acsenergylett.5c00582

Raul A. Marquez, Jay T. Bender, Shashwati C. da Cunha, Ashton M. Aleman, Amaresh Sahu, Venkat Ganesan, Delia J. Milliron, Joaquin Resasco, Thomas F. Jaramillo, C. Buddie Mullins

{"title":"Tracking Local pH Dynamics during Water Electrolysis via In-Line Continuous Flow Raman Spectroscopy","authors":"Raul A. Marquez, Jay T. Bender, Shashwati C. da Cunha, Ashton M. Aleman, Amaresh Sahu, Venkat Ganesan, Delia J. Milliron, Joaquin Resasco, Thomas F. Jaramillo, C. Buddie Mullins","doi":"10.1021/acsenergylett.5c00582","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00582","url":null,"abstract":"The performance of electrochemical devices, which play a critical role in decarbonization efforts, is often governed by proton-coupled electron transfer reactions at the electrode–electrolyte interface. These reactions are highly sensitive to the complex and dynamic microenvironment present at the electrode surface. However, characterizing this environment─particularly monitoring interfacial pH and its evolution under reaction conditions─remains challenging, necessitating the development of advanced analytical tools. Here, we introduce in-line continuous flow Raman spectroscopy (CFRS) as a spectroelectrochemical platform for quantifying interfacial pH swings generated during water-splitting. By monitoring phosphate ion speciation and controlling the hydrodynamics with a flow cell, we measure pH swings as a function of current density, flow rate, and distance from the electrode. Comparison with theoretical models reveals the impact of bulk pH, boundary layer thickness, and bubble dynamics at high current densities. Collectively, these findings establish CFRS as a platform for quantitatively investigating pH dynamics, offering critical insights for advancing electrochemical energy conversion technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"23 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766429","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

Inhibition of CO2 Carbonation Promotes Efficacy of Bicarbonate Electrolysis to CO 抑制CO2碳化可提高碳酸氢盐电解对CO的效率

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-03 DOI: 10.1021/acsenergylett.4c03465

Yingxue Fu, Jun Wu, Hao Chen, Lin Wu, Zhujiang Wang, Fenghua Shen, Kaisong Xiang, Hui Liu

{"title":"Inhibition of CO2 Carbonation Promotes Efficacy of Bicarbonate Electrolysis to CO","authors":"Yingxue Fu, Jun Wu, Hao Chen, Lin Wu, Zhujiang Wang, Fenghua Shen, Kaisong Xiang, Hui Liu","doi":"10.1021/acsenergylett.4c03465","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03465","url":null,"abstract":"The bicarbonate electrolysis process integrates CO2 regeneration with electrolysis, potentially lowering the energy consumption of CO2 conversion. Currently, efforts to elevate the partial current density of target products in bicarbonate electrolysis primarily focus on electrode design and optimization. However, a paradoxical issue is that the activated CO2 (a-CO2) derived from HCO3– tends to reconvert as the current density increases, due to the locally high pH environment. We found that more than 54% of a-CO2 was carbonated in bicarbonate electrolysis at 200 mA cm–2, which led to a reduction in the efficiency of CO2RR. Here, this issue was mitigated by simply introducing buffering additives into the bicarbonate solution. Specifically, with the addition of 20.0 mM ethylenediaminetetraacetic acid (EDTA), the FECO reached 75.3% at 200 mA cm–2, representing a 2.3-fold increase compared to the EDTA-free system. These findings suggest that enhancing buffering capacity is crucial for optimizing bicarbonate electrolysis.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"217 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776192","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

Buried SnI2 Induces Gradient Heterojunctions in Sn–Pb Perovskite Solar Cells 埋藏的SnI2在Sn-Pb钙钛矿太阳能电池中诱导梯度异质结

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-03 DOI: 10.1021/acsenergylett.5c00305

Xuewei Liu, Jia Xu, Chenxu Zhao, Fan Shen, Pengchen Zou, Yijun Wang, Bozhang Ji, Xingjie Guan, Xu Pan, Jianxi Yao

引用次数: 0

Disconnected Lithium Metal Damages Solid-State Electrolytes 断开的锂金属损坏固态电解质

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-02 DOI: 10.1021/acsenergylett.5c00101

Diana Avadanii, Steffen Ganschow, Markus Stypa, Sonja Müller, Sabrina Lang, Dominik Kramer, Christoph Kirchlechner, Reiner Mönig

引用次数: 0

Vacancy-Catalyzed Cation Homogenization for High-Performance AgBiS2 Nanocrystal Solar Cells 空位催化阳离子均匀化制备高性能AgBiS2纳米晶太阳能电池

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-02 DOI: 10.1021/acsenergylett.5c00506

Yang Liu, Zitao Ni, Lucheng Peng, Hao Wu, Zeke Liu, Yongjie Wang, Wanli Ma, Gerasimos Konstantatos

引用次数: 0

Interlayer Cationic Defect Engineering in Lamellar Vanadate Cathodes Enables Ultralong-Lifespan Magnesium-Ion Batteries 层状钒酸盐阴极层间阳离子缺陷工程实现超长寿命镁离子电池

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-02 DOI: 10.1021/acsenergylett.5c00380

Fuyu Chen, Kaifeng Huang, Hong-Yi Li, Qing Zhong, Jili Yue, Jiang Diao, Zhongting Wang, Guangsheng Huang, Bin Jiang, Fusheng Pan

{"title":"Interlayer Cationic Defect Engineering in Lamellar Vanadate Cathodes Enables Ultralong-Lifespan Magnesium-Ion Batteries","authors":"Fuyu Chen, Kaifeng Huang, Hong-Yi Li, Qing Zhong, Jili Yue, Jiang Diao, Zhongting Wang, Guangsheng Huang, Bin Jiang, Fusheng Pan","doi":"10.1021/acsenergylett.5c00380","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00380","url":null,"abstract":"The rate performance and lifespan of rechargeable magnesium-ion batteries (RMIBs) are limited by the low ionic conductivity and poor structural stability of the cathode materials. Herein, we introduce interlayer cationic defect engineering to enhance the diffusion dynamics and structural integrity of vanadate cathodes for the RMIBs. Through interlayer Mg2+ doping, we synthesized a defect-engineered cathode material (d-MgNVO) that establishes optimized migration pathways. Lattice defects confine ionic migration within the vanadate framework and reconstruct short, rapid, and reversible migration pathways, increasing the Mg2+ diffusion coefficient to 10–11–10–13 cm2 s–1. The d-MgNVO cathode exhibits a capacity of 198 mAh g–1 at 0.05 A g–1 and 73 mAh g–1 at 3.0 A g–1, showcasing good rate capability; the PTCDA//d-MgNVO full cell achieves a long lifespan of 5,000 cycles at 1.0 A g–1 with 79% capacity retention. These findings highlight interlayer cationic defect engineering as a promising strategy for high-performance, long-lasting RMIBs and other secondary batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"32 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758594","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

Vacancy-Catalyzed Cation Homogenization for High-Performance AgBiS2 Nanocrystal Solar Cells 空位催化阳离子均匀化制备高性能AgBiS2纳米晶太阳能电池

IF 19.3 1区材料科学

ACS Energy Letters Pub Date : 2025-04-02 DOI: 10.1021/acsenergylett.5c0050610.1021/acsenergylett.5c00506

Yang Liu, Zitao Ni, Lucheng Peng, Hao Wu, Zeke Liu, Yongjie Wang*, Wanli Ma and Gerasimos Konstantatos*,

{"title":"Vacancy-Catalyzed Cation Homogenization for High-Performance AgBiS2 Nanocrystal Solar Cells","authors":"Yang Liu, Zitao Ni, Lucheng Peng, Hao Wu, Zeke Liu, Yongjie Wang*, Wanli Ma and Gerasimos Konstantatos*, ","doi":"10.1021/acsenergylett.5c0050610.1021/acsenergylett.5c00506","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00506https://doi.org/10.1021/acsenergylett.5c00506","url":null,"abstract":"Environmentally friendly silver bismuth sulfide (AgBiS2) nanocrystals (NCs) are promising solution-processed absorbers for photovoltaic applications. Cation disorder nonhomogeneity has been considered as a prevalent obstacle, significantly impacting the optoelectronic properties of AgBiS2 films. In this work, we developed a vacancy-assisted strategy to mitigate the energy barriers for the cation homogenization process in AgBiS2 NC films. Chloride ions are introduced to induce surface vacancies, leading to improved cation homogeneity and enhanced absorption under low-temperature annealing. The resultant AgBiS2 NC solar cells exhibited a power conversion efficiency (PCE) over 10%, the highest to date from a solid-state ligand-exchange method. Our strategy not only enables high-quality AgBiS2 NC films but also provides an approach for engineering cation disorder in multinary materials.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 4","pages":"2068–2074 2068–2074"},"PeriodicalIF":19.3,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143814652","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

Disconnected Lithium Metal Damages Solid-State Electrolytes 断开的锂金属损坏固态电解质

IF 19.3 1区材料科学

ACS Energy Letters Pub Date : 2025-04-02 DOI: 10.1021/acsenergylett.5c0010110.1021/acsenergylett.5c00101

Diana Avadanii*, Steffen Ganschow, Markus Stypa, Sonja Müller, Sabrina Lang, Dominik Kramer, Christoph Kirchlechner and Reiner Mönig*,

{"title":"Disconnected Lithium Metal Damages Solid-State Electrolytes","authors":"Diana Avadanii*, Steffen Ganschow, Markus Stypa, Sonja Müller, Sabrina Lang, Dominik Kramer, Christoph Kirchlechner and Reiner Mönig*, ","doi":"10.1021/acsenergylett.5c0010110.1021/acsenergylett.5c00101","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00101https://doi.org/10.1021/acsenergylett.5c00101","url":null,"abstract":"Solid-state batteries with a lithium–metal anode are energy-storage devices that promise increased energy density and improved safety compared with liquid systems. Despite significant developments, the chemomechanical degradation of solid-state batteries represents a significant challenge to their widespread adoption. Specifically, Li-filled cracks (called “dendrites”) and electronically isolated Li inclusions (“dead” Li) are key defects resulting from coupled electrochemical and mechanical degradation during cycling. In this study, we use a symmetrical Li|LLZO|Li cell with a single-crystal electrolyte and demonstrate that an electronically isolated Li-metal inclusion exhibits bipolarity under an external electrical field, which leads to further crack expansion. We suggest that this process of “dead” metal activation accelerates chemomechanical degradation in solid-state batteries with alkali anodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 4","pages":"2061–2067 2061–2067"},"PeriodicalIF":19.3,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenergylett.5c00101","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143814647","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0