Pub Date : 2024-06-24DOI: 10.1021/acsenergylett.4c01224
Danielle A. Henckel, Prantik Saha, Sunil Rajana, Carlos Baez-Cotto, Audrey K. Taylor, Zengcai Liu, Michael G. Resch, Richard I. Masel, K. C. Neyerlin
Low-temperature electrochemical CO2 reduction has demonstrated high selectivity for CO when devices are operated with pure CO2 streams. However, there is currently a dearth of knowledge for systems operating below 30% CO2, a regime interesting for coupling electrochemical devices with CO2 point sources. Here we examine the influence of ionomer chemistry and cell operating conditions on the CO selectivity at low CO2 concentrations. Utilizing advanced electrochemical diagnostics, values for cathode catalyst layer ionic resistance and electrocatalyst capacitance as a function of relative humidity (RH) were extracted and correlated with selectivity and catalyst utilization. Staying above 20% CO2 concentration with at least a 50% cathode RH resulted in >95% CO/H2 selectivity regardless of the ionomer chemistry. At 10% CO2, however, >95% CO/H2 selectivity was only obtained at 95% RH under scenarios where the resulting electrode morphology enabled high catalyst utilization.
{"title":"Understanding Limitations in Electrochemical Conversion to CO at Low CO2 Concentrations","authors":"Danielle A. Henckel, Prantik Saha, Sunil Rajana, Carlos Baez-Cotto, Audrey K. Taylor, Zengcai Liu, Michael G. Resch, Richard I. Masel, K. C. Neyerlin","doi":"10.1021/acsenergylett.4c01224","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01224","url":null,"abstract":"Low-temperature electrochemical CO<sub>2</sub> reduction has demonstrated high selectivity for CO when devices are operated with pure CO<sub>2</sub> streams. However, there is currently a dearth of knowledge for systems operating below 30% CO<sub>2</sub>, a regime interesting for coupling electrochemical devices with CO<sub>2</sub> point sources. Here we examine the influence of ionomer chemistry and cell operating conditions on the CO selectivity at low CO<sub>2</sub> concentrations. Utilizing advanced electrochemical diagnostics, values for cathode catalyst layer ionic resistance and electrocatalyst capacitance as a function of relative humidity (RH) were extracted and correlated with selectivity and catalyst utilization. Staying above 20% CO<sub>2</sub> concentration with at least a 50% cathode RH resulted in >95% CO/H<sub>2</sub> selectivity regardless of the ionomer chemistry. At 10% CO<sub>2</sub>, however, >95% CO/H<sub>2</sub> selectivity was only obtained at 95% RH under scenarios where the resulting electrode morphology enabled high catalyst utilization.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141448839","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}
Pub Date : 2024-06-20DOI: 10.1021/acsenergylett.4c01095
Yan Liu, Bin Ding, Yong Ding, Gao Zhang, Xin Zhang, Xintong Ma, Yao Wang, Lirong Zeng, Meijun Liu, Guanjun Yang, Mohammad Khaja Nazeeruddin, Bo Chen
Formamidinium lead iodide (FAPbI3) stands out as a promising composition for perovskite solar cells. However, achieving a pure α-FAPbI3 film typically requires a dry environment, which poses a challenge for its widespread commercial application. Our investigation reveals that an excessive presence of dimethyl sulfoxide (DMSO) in the intermediate film obstructs the formation of a pure α-FAPbI3 perovskite film under ambient air. This occurs because DMSO induces instability of intermediates, provokes an unfavorable α-to-δ phase transition, and leaves behind a residual δ-phase in the annealed FAPbI3 film. We discover that there exists a competition between DMSO and MACl regarding the stabilization of the α-phase perovskite structure. A DMSO extraction strategy is proposed to release the beneficial effect of MACl on α-phase stabilization, facilitating the deposition of void-free, pure α-FAPbI3 perovskite films with a low defect density in ambient air. Consequently, this breakthrough enables the fabrication of perovskite solar cells and modules exhibiting impressive efficiencies of 25.71% and 22.12%, respectively.
{"title":"Fabricating α-FAPbI3 Perovskite Photovoltaics in Ambient Air by DMSO Extraction","authors":"Yan Liu, Bin Ding, Yong Ding, Gao Zhang, Xin Zhang, Xintong Ma, Yao Wang, Lirong Zeng, Meijun Liu, Guanjun Yang, Mohammad Khaja Nazeeruddin, Bo Chen","doi":"10.1021/acsenergylett.4c01095","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01095","url":null,"abstract":"Formamidinium lead iodide (FAPbI<sub>3</sub>) stands out as a promising composition for perovskite solar cells. However, achieving a pure α-FAPbI<sub>3</sub> film typically requires a dry environment, which poses a challenge for its widespread commercial application. Our investigation reveals that an excessive presence of dimethyl sulfoxide (DMSO) in the intermediate film obstructs the formation of a pure α-FAPbI<sub>3</sub> perovskite film under ambient air. This occurs because DMSO induces instability of intermediates, provokes an unfavorable α-to-δ phase transition, and leaves behind a residual δ-phase in the annealed FAPbI<sub>3</sub> film. We discover that there exists a competition between DMSO and MACl regarding the stabilization of the α-phase perovskite structure. A DMSO extraction strategy is proposed to release the beneficial effect of MACl on α-phase stabilization, facilitating the deposition of void-free, pure α-FAPbI<sub>3</sub> perovskite films with a low defect density in ambient air. Consequently, this breakthrough enables the fabrication of perovskite solar cells and modules exhibiting impressive efficiencies of 25.71% and 22.12%, respectively.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141430676","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}
Pub Date : 2024-06-20DOI: 10.1021/acsenergylett.4c01281
Majid Safdari, Daehan Kim, Adam Balvanz, Mercouri G. Kanatzidis
Light-induced phase segregation poses challenges for the application of mixed-halide hybrid perovskites in photovoltaics, causing voltage deficits. Here, we investigate the role of chemical composition in improving the photostability of wide bandgap mixed-halide perovskites. We partially substituted the formamidinium cation in the composition of (Cs0.17FA0.83)Pb(Br0.2I0.8)3 with seven alternative cations to achieve a slight blue shift in the bandgap, typically achieved by increasing bromide content. Among alternative cations, dimethylammonium (DMA) and acetamidinium (Ac) induced greater blue shifts at 10% concentration without forming a new low-dimensional second phase. Photoluminescence studies, which analyzed the halide segregation induced by high-power laser irradiation of all new compositions, revealed reduced phase segregation for DMA and Ac compositions. Further adjustments, e.g., increased cesium content, effectively compensated for the lower bromide content in the bandgap while enhancing light stability. Among all compositions, Cs0.25FA0.65DMA0.1Pb(Br0.2I0.8)3 exhibited enhanced photostability. These findings highlight the potential of structural modifications to produce highly stable compositions with the desired bandgap, paving the way for the development of stable perovskite solar cells.
光诱导的相分离给混合卤化物混合包晶在光伏领域的应用带来了挑战，导致电压不足。在此，我们研究了化学成分在改善宽带隙混合卤化物过氧化物光稳定性方面的作用。我们用七种替代阳离子部分取代了 (Cs0.17FA0.83)Pb(Br0.2I0.8)3 组成中的甲脒阳离子，以实现带隙的轻微蓝移，这通常是通过增加溴化物含量来实现的。在替代阳离子中，二甲基铵（DMA）和乙酰氨基铵（Ac）在浓度为 10%时会诱发更大的蓝移，但不会形成新的低维第二相。光致发光研究分析了所有新成分在高功率激光照射下引起的卤化物偏析，发现 DMA 和 Ac 成分的相偏析减少了。进一步的调整，如增加铯的含量，有效地弥补了带隙中溴化物含量的降低，同时提高了光稳定性。在所有成分中，Cs0.25FA0.65DMA0.1Pb(Br0.2I0.8)3 的光稳定性更强。这些发现凸显了结构改性在生产具有所需带隙的高稳定性成分方面的潜力，为开发稳定的过氧化物太阳能电池铺平了道路。
{"title":"Mitigation of Halide Segregation by Cation Composition Management in Wide Bandgap Perovskites","authors":"Majid Safdari, Daehan Kim, Adam Balvanz, Mercouri G. Kanatzidis","doi":"10.1021/acsenergylett.4c01281","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01281","url":null,"abstract":"Light-induced phase segregation poses challenges for the application of mixed-halide hybrid perovskites in photovoltaics, causing voltage deficits. Here, we investigate the role of chemical composition in improving the photostability of wide bandgap mixed-halide perovskites. We partially substituted the formamidinium cation in the composition of (Cs<sub>0.17</sub>FA<sub>0.83</sub>)Pb(Br<sub>0.2</sub>I<sub>0.8</sub>)<sub>3</sub> with seven alternative cations to achieve a slight blue shift in the bandgap, typically achieved by increasing bromide content. Among alternative cations, dimethylammonium (DMA) and acetamidinium (Ac) induced greater blue shifts at 10% concentration without forming a new low-dimensional second phase. Photoluminescence studies, which analyzed the halide segregation induced by high-power laser irradiation of all new compositions, revealed reduced phase segregation for DMA and Ac compositions. Further adjustments, e.g., increased cesium content, effectively compensated for the lower bromide content in the bandgap while enhancing light stability. Among all compositions, Cs<sub>0.25</sub>FA<sub>0.65</sub>DMA<sub>0.1</sub>Pb(Br<sub>0.2</sub>I<sub>0.8</sub>)<sub>3</sub> exhibited enhanced photostability. These findings highlight the potential of structural modifications to produce highly stable compositions with the desired bandgap, paving the way for the development of stable perovskite solar cells.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141430652","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}
Solid-state batteries (SSBs) are considered a promising approach to realizing an anode-free concept with high energy densities. However, the initial Coulombic efficiency (ICE) has remained insufficient for anode-free batteries using sulfide-based solid electrolytes (SEs). Herein, we incorporated a hydride-based interlayer, 3LiBH4-LiI (LBHI), between a typical sulfide SE, Li6PS5Cl, and the Cu current collector. By investigating the Li plating and stripping behaviors and the (electro)chemical stability between SEs and plated Li, we demonstrated that LBHI can effectively improve interfacial stability, leading to an ICE exceeding 94% in anode-free half cells. This interlayer also improves Coulombic efficiencies and specific capacities in anode-free full cells. Furthermore, the utilization of LBHI enables one to study Li plating behaviors without interference from interfacial (electro)chemical instabilities. The analysis of stack pressure evolution during electrochemical cycling reveals that soft shorting in SSBs arises from both dendrite formation and deformation, offering insights into further optimizing solid-state anode-free batteries.
{"title":"Hydride-Based Interlayer for Solid-State Anode-Free Battery","authors":"Yonglin Huang, Yuxuan Zhang, Ruixin Wu, Bowen Shao, Ruihao Deng, Ratnottam Das, Fudong Han","doi":"10.1021/acsenergylett.4c00704","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c00704","url":null,"abstract":"Solid-state batteries (SSBs) are considered a promising approach to realizing an anode-free concept with high energy densities. However, the initial Coulombic efficiency (ICE) has remained insufficient for anode-free batteries using sulfide-based solid electrolytes (SEs). Herein, we incorporated a hydride-based interlayer, 3LiBH<sub>4</sub>-LiI (LBHI), between a typical sulfide SE, Li<sub>6</sub>PS<sub>5</sub>Cl, and the Cu current collector. By investigating the Li plating and stripping behaviors and the (electro)chemical stability between SEs and plated Li, we demonstrated that LBHI can effectively improve interfacial stability, leading to an ICE exceeding 94% in anode-free half cells. This interlayer also improves Coulombic efficiencies and specific capacities in anode-free full cells. Furthermore, the utilization of LBHI enables one to study Li plating behaviors without interference from interfacial (electro)chemical instabilities. The analysis of stack pressure evolution during electrochemical cycling reveals that soft shorting in SSBs arises from both dendrite formation and deformation, offering insights into further optimizing solid-state anode-free batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141435938","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}
Pub Date : 2024-06-14DOI: 10.1021/acsenergylett.4c01391
Marta C. Hatzell*,
{"title":"The Colors of Ammonia","authors":"Marta C. Hatzell*, ","doi":"10.1021/acsenergylett.4c01391","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01391","url":null,"abstract":"","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141322329","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}
Pub Date : 2024-06-14DOI: 10.1021/acsenergylett.4c00843
Xiaozhi Jiang, Fangyan Liu, Maohui Bai, Long Chen, Mengran Wang, Kun Zhang, Jiayi Yang, Bo Hong, Yang Ren, Yanqing Lai, Jie Li
A prevalent method to bolster the safety of lithium-ion batteries (LIBs) is through the deployment of phosphate-based electrolytes. Nonetheless, an intrinsic challenge arises from the incompatibility between phosphate components and graphite anodes, a phenomenon known as coinsertion. To tackle this obstacle, we introduce a comprehensive strategy that employs in situ thermal polymerization, leveraging a flame-retardant solvent and a polymer matrix. This approach fosters strong dipole–dipole interactions between phosphate molecules and the polymer matrix, effectively alleviating the adverse impacts on graphite anodes. This significant enhancement is validated through in situ X-ray diffraction, X-ray photoelectron spectroscopy depth profile analysis, and transmission electron microscopy imaging. Our methodology facilitated stable lithium-ion operations within electrolytes comprising 20% phosphate components in assembled NCM811|P-GPE|Gr pouch cells, achieving a low-capacity decay rate of 0.0023% per cycle with good flame-retardant characteristics. We believe this strategy heralds new commercial prospects for incorporating phosphate-based solvents in the creation of exceptionally safe LIBs.
{"title":"Breaking Solvation Dominance of Phosphate via Dipole–Dipole Chemistry in Gel Polymer Electrolyte","authors":"Xiaozhi Jiang, Fangyan Liu, Maohui Bai, Long Chen, Mengran Wang, Kun Zhang, Jiayi Yang, Bo Hong, Yang Ren, Yanqing Lai, Jie Li","doi":"10.1021/acsenergylett.4c00843","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c00843","url":null,"abstract":"A prevalent method to bolster the safety of lithium-ion batteries (LIBs) is through the deployment of phosphate-based electrolytes. Nonetheless, an intrinsic challenge arises from the incompatibility between phosphate components and graphite anodes, a phenomenon known as coinsertion. To tackle this obstacle, we introduce a comprehensive strategy that employs in situ thermal polymerization, leveraging a flame-retardant solvent and a polymer matrix. This approach fosters strong dipole–dipole interactions between phosphate molecules and the polymer matrix, effectively alleviating the adverse impacts on graphite anodes. This significant enhancement is validated through in situ X-ray diffraction, X-ray photoelectron spectroscopy depth profile analysis, and transmission electron microscopy imaging. Our methodology facilitated stable lithium-ion operations within electrolytes comprising 20% phosphate components in assembled NCM811|P-GPE|Gr pouch cells, achieving a low-capacity decay rate of 0.0023% per cycle with good flame-retardant characteristics. We believe this strategy heralds new commercial prospects for incorporating phosphate-based solvents in the creation of exceptionally safe LIBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141329595","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}
Pub Date : 2024-06-14DOI: 10.1021/acsenergylett.4c00933
Jaeyong Park, Eung-Dab Kim, Sangkuk Kim, Chulwan Lim, Hyunchul Kim, Young-Jin Ko, Jae-Young Choi, Hyung-Suk Oh, Woong Hee Lee
In a membrane electrode assembly (MEA) electrolyzer based on a cation-exchange membrane, achieving an efficient and stable CO2 reduction reaction (CO2RR) is challenging because the transport of protons, cations, and electro-osmotic water from the anode changes the balance of ions. Herein, we derived a microenvironment for stable and efficient CO2RR performance by using two strategies. First, a mixture of carbon and anion-exchange ionomer buffer layers is used to hold cations while managing water in local alkaline media. The second strategy involves pressurizing only the cathode side, resulting in a high local CO2 concentration and enhancing the reverse osmosis phenomenon. The synergistic effects of these two strategies create an efficient microenvironment by managing water and cations, leading to a stable and efficient CO2RR operation. Our approach of reverse osmosis to balance cations and water is viable for industrial applications because pressurized CO2 and MEA systems are efficient processes that can be commercialized.
在基于阳离子交换膜的膜电极组件（MEA）电解槽中，实现高效稳定的二氧化碳还原反应（CO2RR）具有挑战性，因为质子、阳离子和电渗水从阳极的传输会改变离子的平衡。在此，我们采用两种策略，得出了一种可实现稳定、高效 CO2RR 性能的微环境。首先，使用碳和阴离子交换离子聚合物缓冲层的混合物来保持阳离子，同时管理局部碱性介质中的水。第二种策略是只对阴极一侧加压，从而产生较高的局部二氧化碳浓度，并增强反渗透现象。这两种策略的协同效应通过管理水和阳离子创造了一个高效的微环境，从而实现了稳定高效的 CO2RR 运行。我们利用反渗透来平衡阳离子和水的方法在工业应用中是可行的，因为加压二氧化碳和 MEA 系统是可以商业化的高效工艺。
{"title":"Deriving an Efficient and Stable Microenvironment for a CO2 MEA Electrolyzer by Reverse Osmosis","authors":"Jaeyong Park, Eung-Dab Kim, Sangkuk Kim, Chulwan Lim, Hyunchul Kim, Young-Jin Ko, Jae-Young Choi, Hyung-Suk Oh, Woong Hee Lee","doi":"10.1021/acsenergylett.4c00933","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c00933","url":null,"abstract":"In a membrane electrode assembly (MEA) electrolyzer based on a cation-exchange membrane, achieving an efficient and stable CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) is challenging because the transport of protons, cations, and electro-osmotic water from the anode changes the balance of ions. Herein, we derived a microenvironment for stable and efficient CO<sub>2</sub>RR performance by using two strategies. First, a mixture of carbon and anion-exchange ionomer buffer layers is used to hold cations while managing water in local alkaline media. The second strategy involves pressurizing only the cathode side, resulting in a high local CO<sub>2</sub> concentration and enhancing the reverse osmosis phenomenon. The synergistic effects of these two strategies create an efficient microenvironment by managing water and cations, leading to a stable and efficient CO<sub>2</sub>RR operation. Our approach of reverse osmosis to balance cations and water is viable for industrial applications because pressurized CO<sub>2</sub> and MEA systems are efficient processes that can be commercialized.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141329495","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}
Pub Date : 2024-06-14DOI: 10.1021/acsenergylett.4c01390
Kelsey B. Hatzell, Prashant V. Kamat
Figure 1. Schematics of a Li-garnet solid state battery. Reproduced with permission from ref [10]. Copyright American Chemical Society. This article has not yet been cited by other publications. Figure 1. Schematics of a Li-garnet solid state battery. Reproduced with permission from ref [10]. Copyright American Chemical Society.
{"title":"Tutorials in Electrochemistry: Storage Batteries","authors":"Kelsey B. Hatzell, Prashant V. Kamat","doi":"10.1021/acsenergylett.4c01390","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01390","url":null,"abstract":"Figure 1. Schematics of a Li-garnet solid state battery. Reproduced with permission from ref [10]. Copyright American Chemical Society. This article has not yet been cited by other publications. Figure 1. Schematics of a Li-garnet solid state battery. Reproduced with permission from ref [10]. Copyright American Chemical Society.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141329548","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}
Pub Date : 2024-06-14DOI: 10.1021/acsenergylett.4c00271
Hiba Saada, Bruno Fabre, Gabriel Loget, Gwenaëlle Benoit
Dihydrogen (H2) constitutes a promising energy carrier for transporting part of the world’s energy demand and concomitantly for reducing toxic emissions. Water electrolysis powered by renewable energy would provide H2 with a small carbon footprint. To save global fresh water, seawater electrolysis has attracted much attention in recent years, since it represents 96.5% of the Earth’s resources and is abundant worldwide. However, seawater’s composition is complex, which poses problems for direct seawater splitting. To date, seawater splitting usually requires a two-step process, i.e., purification of seawater using reverse osmosis (RO) which represents 69% of the globally produced desalinated water (Jones et al. Sci. Total Environ.2019, 657, 1343–1356) and then electrolysis of pure water. This involves two separate processes, resulting in a complex design and significant space requirement for their corresponding equipment. Recently, efforts have been made to use seawater directly for H2 production, and electrolyzers using this water source are being developed. The objective of this review is to describe first the impact of direct seawater splitting on water electrolysis technologies and then to present the most recent innovative approaches to avoid pretreatment with particular emphasis on innovative configurations of well-established industrial electrolyzers and new original approaches. Finally, as a conclusion, we will propose perspectives toward the development of electrolyzers enabling the electrochemical production of H2 from seawater for sustainable development.
{"title":"Is Direct Seawater Splitting Realistic with Conventional Electrolyzer Technologies?","authors":"Hiba Saada, Bruno Fabre, Gabriel Loget, Gwenaëlle Benoit","doi":"10.1021/acsenergylett.4c00271","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c00271","url":null,"abstract":"Dihydrogen (H<sub>2</sub>) constitutes a promising energy carrier for transporting part of the world’s energy demand and concomitantly for reducing toxic emissions. Water electrolysis powered by renewable energy would provide H<sub>2</sub> with a small carbon footprint. To save global fresh water, seawater electrolysis has attracted much attention in recent years, since it represents 96.5% of the Earth’s resources and is abundant worldwide. However, seawater’s composition is complex, which poses problems for direct seawater splitting. To date, seawater splitting usually requires a two-step process, i.e., purification of seawater using reverse osmosis (RO) which represents 69% of the globally produced desalinated water (Jones et al. <i>Sci. Total Environ.</i> <b>2019</b>, <i>657</i>, 1343–1356) and then electrolysis of pure water. This involves two separate processes, resulting in a complex design and significant space requirement for their corresponding equipment. Recently, efforts have been made to use seawater directly for H<sub>2</sub> production, and electrolyzers using this water source are being developed. The objective of this review is to describe first the impact of direct seawater splitting on water electrolysis technologies and then to present the most recent innovative approaches to avoid pretreatment with particular emphasis on innovative configurations of well-established industrial electrolyzers and new original approaches. Finally, as a conclusion, we will propose perspectives toward the development of electrolyzers enabling the electrochemical production of H<sub>2</sub> from seawater for sustainable development.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141329594","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}
The chaotropic salt electrolyte (CSE) has become an effective strategy to activate low-temperature aqueous zinc-ion batteries. However, the Zn battery performance has been largely compromised due to the side reaction of active water molecules in CSE. Herein we design a Zn(BF4)2 in a propylene carbonate–water cosolvent electrolyte that facilitates the zinc plating/stripping in a wide temperature range (−40 to 60 °C). Theoretical and experimental results demonstrate the dual effect of propylene carbonate on regulating the hydrogen bond network and reshaping the Zn2+ solvation structure, bringing the antifreezing property and smooth Zn plating/stripping. Consequently, at −20 °C, the Cu//Zn asymmetric cell can achieve stable cycling for over 4000 h at 0.5 mAh cm–2. At −40 °C, the Zn//tetrachlorobenzoquinone full battery can deliver a reversible specific capacity of 77.9 mAh g–1 after 700 cycles. This work presents an effective strategy for the development of high-performance ZIBs in a wide temperature range.
{"title":"Carbonate-Assisted Chaotropic Electrolyte for Zinc Ion Battery with Wide Temperature Operation","authors":"Zehui Xie, Na Chen, Mingjun Zhang, Mingming Wang, Xinhua Zheng, Shuang Liu, Ruihao Luo, Li Song, Yahan Meng, Zaichun Liu, Zhenyu Li, Wei Chen","doi":"10.1021/acsenergylett.4c00833","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c00833","url":null,"abstract":"The chaotropic salt electrolyte (CSE) has become an effective strategy to activate low-temperature aqueous zinc-ion batteries. However, the Zn battery performance has been largely compromised due to the side reaction of active water molecules in CSE. Herein we design a Zn(BF<sub>4</sub>)<sub>2</sub> in a propylene carbonate–water cosolvent electrolyte that facilitates the zinc plating/stripping in a wide temperature range (−40 to 60 °C). Theoretical and experimental results demonstrate the dual effect of propylene carbonate on regulating the hydrogen bond network and reshaping the Zn<sup>2+</sup> solvation structure, bringing the antifreezing property and smooth Zn plating/stripping. Consequently, at −20 °C, the Cu//Zn asymmetric cell can achieve stable cycling for over 4000 h at 0.5 mAh cm<sup>–2</sup>. At −40 °C, the Zn//tetrachlorobenzoquinone full battery can deliver a reversible specific capacity of 77.9 mAh g<sup>–1</sup> after 700 cycles. This work presents an effective strategy for the development of high-performance ZIBs in a wide temperature range.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141333839","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}
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