JoulePub Date : 2025-03-27DOI: 10.1016/j.joule.2025.101885
Yawei Chen, Menghao Li, Yulin Jie, Yue Liu, Zhengfeng Zhang, Peiping Yu, Wanxia Li, Yang Liu, Xinpeng Li, Zhanwu Lei, Pengfei Yan, Tao Cheng, M. Danny Gu, Shuhong Jiao, Ruiguo Cao
{"title":"Dynamic evolution of cathode-electrolyte interphase in lithium metal batteries with ether electrolytes","authors":"Yawei Chen, Menghao Li, Yulin Jie, Yue Liu, Zhengfeng Zhang, Peiping Yu, Wanxia Li, Yang Liu, Xinpeng Li, Zhanwu Lei, Pengfei Yan, Tao Cheng, M. Danny Gu, Shuhong Jiao, Ruiguo Cao","doi":"10.1016/j.joule.2025.101885","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101885","url":null,"abstract":"High-voltage lithium (Li) metal batteries (HVLMBs) have attracted tremendous research interest in the past decade owing to their high energy densities. Electrode-electrolyte interphases in HVLMBs play critical roles in dictating their electrochemical performance. However, despite the intensive research on solid-electrolyte interphase (SEI) of Li anode, the cathode-electrolyte interphase (CEI) on high-voltage cathodes remains elusive. Herein, we report the formation and dynamic evolution of CEI on LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811) cathodes in ether-based electrolytes. We reveal that the solvent-derived interphase predominates the initial CEI, which subsequently evolves into a Li fluoride (LiF)-rich CEI during cycling. Through solvent design, the weak-solvation electrolyte with branched ether solvents promotes the formation of a conformal CEI layer featuring the monodispersing LiF nanocrystals (∼8 nm), thereby enabling NMC811 cathodes to sustain up to 2,000 cycles. This work addresses the long-standing questions regarding CEI evolution and provides valuable guidance for the rational electrolyte design for HVLMBs.","PeriodicalId":343,"journal":{"name":"Joule","volume":"133 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713656","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}
JoulePub Date : 2025-03-26DOI: 10.1016/j.joule.2025.101883
Bei Zhou, Hengzhou Liu, Guangcan Su, Heejong Shin, Xiao-Yan Li, Huajie Ze, Yongxiang Liang, Bosi Peng, Weiyan Ni, Yuanjun Chen, Wenjin Zhu, Christine Yu, Yiqing Chen, Pengfei Ou, Ke Xie, Edward H. Sargent
{"title":"Electrosynthesis of CO from an electrically pH-shifted DAC post-capture liquid using a catalyst:support amide linkage","authors":"Bei Zhou, Hengzhou Liu, Guangcan Su, Heejong Shin, Xiao-Yan Li, Huajie Ze, Yongxiang Liang, Bosi Peng, Weiyan Ni, Yuanjun Chen, Wenjin Zhu, Christine Yu, Yiqing Chen, Pengfei Ou, Ke Xie, Edward H. Sargent","doi":"10.1016/j.joule.2025.101883","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101883","url":null,"abstract":"Electrified reactive capture upgrades CO<sub>2</sub> from post-air-capture alkali carbonate liquid to value-added products while regenerating the capture medium. Previous processes exhibited limited energy efficiency (<18%) due to high full-cell voltage (>3.7 V) and modest CO selectivity (<45%). To address this, we developed a Co molecular catalyst featuring an electron-deficient Co center, lowering the required reduction voltage. We then grafted the catalyst onto a conductive support, enhancing charge transfer. An electrified pH-downshifter improved CO<sub>2</sub> availability, increasing CO selectivity. The system achieved 70% CO selectivity at 2.7 V and 100 mA cm<sup>−2</sup>, corresponding to an energy intensity of 35 GJ/ton CO. The energy cost is comparable to that of direct air capture (DAC) followed by reverse water-gas shift (RWGS), but it offers ambient temperature operation.","PeriodicalId":343,"journal":{"name":"Joule","volume":"99 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703354","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}
{"title":"Variable and intelligent catalyst design based on local chemical environments in sulfur redox reactions","authors":"Yeyang Jia, Zhilong Wang, Zhiyuan Han, Junfeng Li, Mengtian Zhang, Zhoujie Lao, Yanqiang Han, Runhua Gao, Jing Gao, Zhiyang Zheng, An Chen, Hong Li, Rui Mao, Kehao Tao, Jinjin Li, Guangmin Zhou","doi":"10.1016/j.joule.2025.101878","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101878","url":null,"abstract":"The conventional constant catalyst design approach demonstrates limited adaptability to external conditions, impairing the catalytic performance in practical lithium-sulfur (Li-S) batteries. Here, we propose a variable and intelligent catalyst design strategy based on catalysts’ local chemical environments (LCEs). The competing adsorption between polysulfides and solvents within LCEs governs the interfacial reactions, regulated by the interaction between extrinsic electrolyte effects and intrinsic catalyst structures. Using nickel sulfides as a model system, interpretable machine-learning methods provide intelligent insights into structural tuning. Reversed catalytic efficiency is observed in LCEs of diluted and concentrated polysulfides, and variable catalyst modification guidance is presented for accelerating electron and ion transfer rates, respectively. Li-S batteries based on a Ni<sub>3</sub>S<sub>2</sub> catalyst manifest exceptional performance in a lean electrolyte, achieving an energy density of 433 Wh kg<sup>−1</sup> in pouch cells. This investigation provides a thorough design protocol for catalysts and promotes practical applications of Li-S batteries through catalytic conversion.","PeriodicalId":343,"journal":{"name":"Joule","volume":"32 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143666091","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}
JoulePub Date : 2025-03-19DOI: 10.1016/j.joule.2024.12.001
Yongxi Li , Karthik Kamaraj , Yogita Silori , Haonan Zhao , Claire Arneson , Bin Liu , Jennifer Ogilvie , Stephen R. Forrest
{"title":"Radiation hardness of organic photovoltaics","authors":"Yongxi Li , Karthik Kamaraj , Yogita Silori , Haonan Zhao , Claire Arneson , Bin Liu , Jennifer Ogilvie , Stephen R. Forrest","doi":"10.1016/j.joule.2024.12.001","DOIUrl":"10.1016/j.joule.2024.12.001","url":null,"abstract":"<div><div>We investigate the resilience of organic photovoltaic (OPV) cells to proton irradiation at doses equivalent to that experienced by spacecraft in low earth orbit. The OPVs, with their inherent flexibility, light weight, low temperature processing, and potential to achieve high specific power of 40 W/g, are promising candidates for energy production in space. However, their ability to withstand irradiation by high-energy incident radiation and subatomic particles characteristic of harsh space environments is yet unproven. We find that small-molecule OPVs grown by vacuum thermal evaporation are resistant to degradation by 30 keV proton irradiation, in contrast to polymer-based OPVs that suffer a 50% efficiency loss under similar conditions. Thermal annealing at low temperatures significantly restores the polymer-based OPV power conversion efficiency. The loss of efficiency is attributed to cleavage of pendant alkyl groups on the polymers, resulting in cross-linking and the subsequent formation of deep electronic traps.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 3","pages":"Article 101800"},"PeriodicalIF":38.6,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142937354","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}
JoulePub Date : 2025-03-19DOI: 10.1016/j.joule.2024.12.007
Dayin He , Xianhui Ma , Huang Zhou , Yu Zhang , Yuen Wu
{"title":"Continuous conversion of flue gas into syngas by a bipolar membrane-integrated single-cell cyclic system","authors":"Dayin He , Xianhui Ma , Huang Zhou , Yu Zhang , Yuen Wu","doi":"10.1016/j.joule.2024.12.007","DOIUrl":"10.1016/j.joule.2024.12.007","url":null,"abstract":"<div><div>Electrochemical CO<sub>2</sub> reduction reaction (ECO<sub>2</sub>RR) usually requires high-purity CO<sub>2</sub> gas feeding. However, capturing CO<sub>2</sub> from flue gas is still a cost- and energy-intensive process. Here, we design a bipolar membrane-integrated single-cell cyclic system that directly converts simulated flue gas into syngas. The system features a circulating gas-liquid mixed flow between the anode and cathode in an integrated cell, enabling it to simultaneously absorb CO<sub>2</sub> from flue gas and convert captured CO<sub>2</sub> into syngas. At an industrial current density of 250 mA/cm<sup>2</sup>, we successfully decrease the CO<sub>2</sub> concentration in flue gas from 15% to 4.3% (with a 61.7% CO<sub>2</sub> capture efficiency) and obtain high-selectivity (up to 100%) syngas (H<sub>2</sub>:CO = 3:1). Moreover, this cell has excellent tolerance to SO<sub>x</sub> and NO<sub>x</sub> due to the Ni single-atom catalyst in the cathode compared with previous studies. These results pave the way for low-concentration carbon dioxide conversion and promote the application of ECO<sub>2</sub>RR technology.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 3","pages":"Article 101806"},"PeriodicalIF":38.6,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142939527","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}
JoulePub Date : 2025-03-19DOI: 10.1016/j.joule.2024.101815
Deng Wang , Zhixin Liu , Ying Qiao , Zhengyan Jiang , Peide Zhu , Jie Zeng , Wenbo Peng , Qing Lian , Geping Qu , Yintai Xu , Yong Zhang , Fengzhu Li , Lei Yan , Xingzhu Wang , Yang-Gang Wang , Alex K.-Y. Jen , Baomin Xu
{"title":"Rigid molecules anchoring on NiOx enable >26% efficiency perovskite solar cells","authors":"Deng Wang , Zhixin Liu , Ying Qiao , Zhengyan Jiang , Peide Zhu , Jie Zeng , Wenbo Peng , Qing Lian , Geping Qu , Yintai Xu , Yong Zhang , Fengzhu Li , Lei Yan , Xingzhu Wang , Yang-Gang Wang , Alex K.-Y. Jen , Baomin Xu","doi":"10.1016/j.joule.2024.101815","DOIUrl":"10.1016/j.joule.2024.101815","url":null,"abstract":"<div><div>The surface defects of nickel oxide (NiO<sub>x</sub>) and its interfacial redox reactions with perovskites often impede the efficiency improvement of inverted perovskite solar cells (PSCs). To address these issues, we designed ((9H-fluoren-9-ylidene)methyl) cyanophosphonic acid (FY-CPA) with a rigid backbone as an optimal multi-dentate anchoring (MDA) molecule to enhance the anchorage with bottom NiO<sub>x</sub> by forming tetradentate binding and parallel orientation. Dense and uniform coverage of FY-CPA at the NiO<sub>x</sub>/perovskite interface was achieved through <em>in situ</em> deposition, which can minimize interfacial redox reactions and suppress non-radiative recombination. The champion device demonstrated a power conversion efficiency (PCE) of 26.21% with a certified value of 25.99%. In addition, the larger area device (1.02 cm<sup>2</sup>) also showed a PCE of 25.31% with a certified value of 24.90%, which is among the highest PCEs reported so far for greater than 1 cm<sup>2</sup> sized PSCs. Moreover, the as-prepared device exhibited enhanced thermal and operational stability during long-term storage.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 3","pages":"Article 101815"},"PeriodicalIF":38.6,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026800","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}
JoulePub Date : 2025-03-19DOI: 10.1016/j.joule.2024.101816
Haoxuan Liu (刘昊轩) , Zongxu Zhang (张宗旭) , Yating Shi (史娅婷) , Wei Ran (冉玮) , Hua Zhong (仲华) , Fei Zhang (张飞)
{"title":"A low-cost and bendable “cage” for stable rigid and flexible perovskite solar cells with negligible lead leakage","authors":"Haoxuan Liu (刘昊轩) , Zongxu Zhang (张宗旭) , Yating Shi (史娅婷) , Wei Ran (冉玮) , Hua Zhong (仲华) , Fei Zhang (张飞)","doi":"10.1016/j.joule.2024.101816","DOIUrl":"10.1016/j.joule.2024.101816","url":null,"abstract":"<div><div>Research on reducing lead (Pb) leakage in flexible and rigid perovskite solar cells (PSCs) simultaneously is limited, with issues including high material cost or low adsorption efficiency. In this study, we developed a cost-effective (0.8 $/m<sup>2</sup>) and flexible mercaptosuccinic acid-modified polyvinyl alcohol (MMP) film with high Pb-adsorption capacity for rigid and flexible substrates. The formed ester and thiol groups binding to Pb<sup>2+</sup> endowed the MMP film with excellent Pb-adsorption capacity. Combined with polydimethylsiloxane (PDMS), the PDMS-MMP film enabled a Pb sequestration efficiency (SQE) of 99% for rigid and flexible PSCs and modules, with no negative impact on their performance, operational stability and bending stability. This is the first study to achieve a 99% SQE in rigid and flexible PSCs and modules at a low cost, marking a significant advancement toward the safe commercialization of perovskite photovoltaic products.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 3","pages":"Article 101816"},"PeriodicalIF":38.6,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044625","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}
JoulePub Date : 2025-03-19DOI: 10.1016/j.joule.2025.101870
Shuangyan Hu , Wanli Li , Shunchang Liu , Zhiwen Zhou , Yaokang Zhang , Ziqing Luo , Huanyu Jin , Qun Jin , Yi Hou , Xuechang Zhou , Zaiwei Wang
{"title":"Flexible perovskite-based multiple-junction photovoltaics","authors":"Shuangyan Hu , Wanli Li , Shunchang Liu , Zhiwen Zhou , Yaokang Zhang , Ziqing Luo , Huanyu Jin , Qun Jin , Yi Hou , Xuechang Zhou , Zaiwei Wang","doi":"10.1016/j.joule.2025.101870","DOIUrl":"10.1016/j.joule.2025.101870","url":null,"abstract":"<div><div>Flexible solar cells with competitive power-per-weight can be utilized in portable electric chargers, building-integrated photovoltaics, power sources for unmanned aerial vehicles, space-deployable solar arrays, and so on. Multiple-junction flexible solar cells present a promising pathway to surpass the theoretical Shockley-Queisser single-junction limit (33%). Perovskites are ideal photosensitive materials for multiple-junction flexible solar cells. Lead-based halide perovskites can be employed as ideal absorbers in middle- or wide-band-gap subcells, and flexible narrow-band-gap absorbers like lead-tin mixed perovskites, Cu(In, Ga)(S, Se)<sub>2</sub>, organic semiconductors, and Si are compelling candidates for bottom subcells in perovskite-based multiple-junction flexible solar cells. In this review, we summarize the progress made so far; provide an outlook on potential device configurations; discuss strategies to overcome related challenges; and offer a perspective on configuration design, material choice, encapsulation, and scalable fabrication of perovskite-based multiple-junction flexible solar cells.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 3","pages":"Article 101870"},"PeriodicalIF":38.6,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143582483","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}
JoulePub Date : 2025-03-19DOI: 10.1016/j.joule.2025.101875
Regina García-Méndez
{"title":"Engineering stable interphases with multi-salt electrolytes","authors":"Regina García-Méndez","doi":"10.1016/j.joule.2025.101875","DOIUrl":"10.1016/j.joule.2025.101875","url":null,"abstract":"<div><div>Electrode interphases are vital for energy storage performance, regulating ion transport and preventing side reactions. In a recent <em>Journal of the American Chemical Society</em> study, Wang et al. investigated how multi-salt electrolytes form stable, inorganic-rich interphases that enhance ionic transport, cycling efficiency, rate capability, and durability.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 3","pages":"Article 101875"},"PeriodicalIF":38.6,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143645104","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}
JoulePub Date : 2025-03-19DOI: 10.1016/j.joule.2025.101820
Tao Xiao , Lingli Liu , Huan Liu , Ting Li , Daqian Cai , Wen Siang Lew , Yongqi Zhang , Haoming Bao , Jin-Lin Yang , Hong Jin Fan
{"title":"Highly rechargeable aqueous Sn-metal-based hybrid-ion batteries","authors":"Tao Xiao , Lingli Liu , Huan Liu , Ting Li , Daqian Cai , Wen Siang Lew , Yongqi Zhang , Haoming Bao , Jin-Lin Yang , Hong Jin Fan","doi":"10.1016/j.joule.2025.101820","DOIUrl":"10.1016/j.joule.2025.101820","url":null,"abstract":"<div><div>Tin (Sn) metal, with its intrinsic resistance to the hydrogen evolution reaction (HER), holds great promise as an anode for safe and rechargeable aqueous Sn-metal batteries (ASBs). However, the major challenges for their practical deployment include uneven Sn deposition and low Sn<sup>2+</sup>/Sn<sup>4+</sup> reaction reversibility. To mitigate these challenges, we design ASBs from both anode and electrolyte. First, a stannophilic silver-coated vertical graphene (Ag-VG) host improves the nucleation kinetics and uniform Sn deposition. Second, a biphasic H<sub>2</sub>O/ionic liquid (IL) electrolyte confines Sn<sup>2+</sup> within the aqueous phase, suppressing the formation of Sn<sup>4+</sup> at the cathode side and eliminating the usage of an ion exchange membrane. The biphasic electrolyte and Ag-VG host are coupled with various types of cathodes (herein, halogens, LiCoO<sub>2</sub>, and Li<sub>2</sub>MnO<sub>4</sub>) to fabricate full ASBs. Improved cycling stability and Coulombic efficiency are clearly observed. This work highlights a facile strategy for advancing ASBs.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 3","pages":"Article 101820"},"PeriodicalIF":38.6,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143072099","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}