eSciencePub Date : 2023-08-01DOI: 10.1016/j.esci.2023.100141
Xia Wang , Minghao Yu , Xinliang Feng
{"title":"Electronic structure regulation of noble metal-free materials toward alkaline oxygen electrocatalysis","authors":"Xia Wang , Minghao Yu , Xinliang Feng","doi":"10.1016/j.esci.2023.100141","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100141","url":null,"abstract":"<div><p>Developing highly efficient, inexpensive catalysts for oxygen electrocatalysis in alkaline electrolytes (i.e., the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER)) is essential for constructing advanced energy conversion techniques (such as electrolyzers, fuel cells, and metal–air batteries). Recent achievements in efficient noble metal-free ORR and OER catalysts make the replacement of conventional noble metal counterparts a realistic possibility. In particular, various electronic structure regulation strategies have been employed to endow these oxygen catalysts with attractive physicochemical properties and strong synergistic effects, providing significant fundamental understanding to advance in this direction. This review article summarizes recently developed electronic structure regulation strategies for three types of noble metal-free oxygen catalysts: transition metal compounds, single-atom catalysts, and metal-free catalysts. We begin by briefly presenting the basic ORR and OER reaction mechanisms, following this with an analysis of the fundamental relationship between electronic structure and intrinsic electrocatalytic activity for the three categories of catalysts. Subsequently, recent advances in electronic structure regulation strategies for noble metal-free ORR and OER catalysts are systematically discussed. We conclude by summarizing the remaining challenges and presenting our outlook on the future for designing and synthesizing noble metal-free oxygen electrocatalysts.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"3 4","pages":"Article 100141"},"PeriodicalIF":0.0,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49879075","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
eSciencePub Date : 2023-06-01DOI: 10.1016/j.esci.2023.100117
Liang Hu , Bingzhang Yang , Zhipeng Hou , Yangfan Lu , Weitao Su , Lingwei Li
{"title":"Unlocking the charge doping effect in softly intercalated ultrathin ferromagnetic superlattice","authors":"Liang Hu , Bingzhang Yang , Zhipeng Hou , Yangfan Lu , Weitao Su , Lingwei Li","doi":"10.1016/j.esci.2023.100117","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100117","url":null,"abstract":"<div><p>The electrolyte-assisted exfoliation strategy is widely employed to synthesize ultrathin two-dimensional (2D) materials. Yet, spins in 2D magnets are susceptible to the electrolyte due to the underlying charge doping effect. Hence, it is crucial to understand and trace the doping process during the delamination of 2D magnets. Taking the prototype Fe<sub>3</sub>GeTe<sub>2</sub>, we utilized soft organic cations to exfoliate the bulk and obtain a freestanding organic–inorganic hybrid superlattice with a giant electron doping effect as high as 6.9 × 10<sup>14</sup>/cm<sup>2</sup> (∼1.15 electrons per formula unit). A remarkable ferromagnetic transition exceeding 385 K was revealed in these superlattices, together with unique anisotropic saturation magnetization. The doping enhanced the in-plane electron–phonon coupling and thus optimized originally poor indirect double-exchange scenario for spin electrons. The emerging vertical magnetization shift phenomenon served to evaluate the uniformity of charge doping. The above findings provide a new perspective for understanding the role of parasitic charge in 2D magnetism.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"3 3","pages":"Article 100117"},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49884204","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
eSciencePub Date : 2023-06-01DOI: 10.1016/j.esci.2023.100115
Qi Zou , Jin Qiu , Yaping Zang , He Tian , Latha Venkataraman
{"title":"Modulating single-molecule charge transport through external stimulus","authors":"Qi Zou , Jin Qiu , Yaping Zang , He Tian , Latha Venkataraman","doi":"10.1016/j.esci.2023.100115","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100115","url":null,"abstract":"<div><p>Understanding and tuning charge transport over a single molecule is a fundamental topic in molecular electronics. Single-molecule junctions composed of individual molecules attached to two electrodes are the most common components built for single-molecule charge transport studies. During the past two decades, rapid technical and theoretical advances in single-molecule junctions have increased our understanding of the conductance properties and functions of molecular devices. In this perspective article, we introduce the basic principles of charge transport in single-molecule junctions, then give an overview of recent progress in modulating single-molecule transport through external stimuli such as electric field and potential, light, mechanical force, heat, and chemical environment. Lastly, we discuss challenges and offer views on future developments in molecular electronics.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"3 3","pages":"Article 100115"},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49884199","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
eSciencePub Date : 2023-06-01DOI: 10.1016/j.esci.2023.100110
Jiao Lin , Xu Chen , Ersha Fan , Xiaodong Zhang , Renjie Chen , Feng Wu , Li Li
{"title":"A green repair pathway for spent spinel cathode material: Coupled mechanochemistry and solid-phase reactions","authors":"Jiao Lin , Xu Chen , Ersha Fan , Xiaodong Zhang , Renjie Chen , Feng Wu , Li Li","doi":"10.1016/j.esci.2023.100110","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100110","url":null,"abstract":"<div><p>A way of directly repairing spent lithium-ion battery cathode materials is needed in response to environmental pollution and resource depletion. In this work, we report a green repair method involving coupled mechanochemistry and solid-state reactions for spent lithium-ion batteries. During the ball-milling repair process, an added manganese source enters into the degraded LiMn<sub>2</sub>O<sub>4</sub> (LMO) crystal structure in order to fill the Mn vacancies formed by Mn deficiency due to the Jahn–Teller effect, thereby repairing the LMO's chemical composition. An added carbon source acts not only as a lubricant but also as a conductor to improve the material's electrical conductivity. Meanwhile, mechanical force reduces the crystal size of the LMO particles, increasing the amount of active sites for electrochemical reactions. Jahn–Teller distortion is successfully suppressed by cation disorder in the LMO material. The cycling stability and rate performance of the repaired cathode material are thereby greatly improved, with the discharge specific capacity being more than twice that of commercial LMO. The proposed solid-state mechanochemical in situ repair process, which is safe for the environment and simple to use, may be extended to the repair of other waste materials without consuming highly acidic or alkaline chemical reagents.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"3 3","pages":"Article 100110"},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49883647","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
eSciencePub Date : 2023-06-01DOI: 10.1016/j.esci.2023.100120
Shuang Wu , Zhenglin Hu , Pan He , Lingxiao Ren , Jiaxing Huang , Jiayan Luo
{"title":"Crystallographic engineering of Zn anodes for aqueous batteries","authors":"Shuang Wu , Zhenglin Hu , Pan He , Lingxiao Ren , Jiaxing Huang , Jiayan Luo","doi":"10.1016/j.esci.2023.100120","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100120","url":null,"abstract":"<div><p>With their intrinsic safety and environmental benignity, aqueous Zn-ion batteries (ZIBs) have been considered the most appropriate candidates for replacing alkali metal systems. However, polycrystalline Zn anodes in aqueous environments still pose enormous issues, such as dendrite growth and side reactions. Although many efforts have been made to address these obstacles through interphase modification and electrolyte design, researchers have not been able to improve the inherent thermodynamic stability and ion deposition behavior of the Zn anode. It is imperative to understand and explore advanced anode construction methods from the perspective of crystallinity. This review delves into the feasibility of precisely regulating the crystallographic features of metallic zinc, examines the challenges and merits of reported strategies for fabricating textured zinc, and offers constructive suggestions for the large-scale production and commercial application of aqueous ZIBs.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"3 3","pages":"Article 100120"},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49884200","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
eSciencePub Date : 2023-06-01DOI: 10.1016/j.esci.2023.100122
Tianyi Cao , Xiao-Lei Shi , Meng Li , Boxuan Hu , Wenyi Chen , Wei-Di Liu , Wanyu Lyu , Jennifer MacLeod , Zhi-Gang Chen
{"title":"Advances in bismuth-telluride-based thermoelectric devices: Progress and challenges","authors":"Tianyi Cao , Xiao-Lei Shi , Meng Li , Boxuan Hu , Wenyi Chen , Wei-Di Liu , Wanyu Lyu , Jennifer MacLeod , Zhi-Gang Chen","doi":"10.1016/j.esci.2023.100122","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100122","url":null,"abstract":"<div><p>By effectively converting waste heat into electricity, thermoelectric materials and devices can provide an alternative approach to tackle the energy crisis. Amongst thermoelectric materials, bismuth telluride (Bi<sub>2</sub>Te<sub>3</sub>) and its derivatives exhibit high figure of merit <em>ZT</em> values in the near-room-temperature region and show great potential for application in thermoelectric devices. Considering the rapid development of Bi<sub>2</sub>Te<sub>3</sub>-based thermoelectric materials and their devices in the last few years, a short and systematic review is much needed. Here, we summarize the novel designs, properties, and applications of Bi<sub>2</sub>Te<sub>3</sub>-based thermoelectric devices in different contexts, including wearable, portable, implantable, and cross-disciplinary applications. The challenges and outlook for Bi<sub>2</sub>Te<sub>3</sub>-based thermoelectric devices are also considered. This work will guide the future development of Bi<sub>2</sub>Te<sub>3</sub>-based thermoelectric devices that target broader and more practical applications.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"3 3","pages":"Article 100122"},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49884203","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
eSciencePub Date : 2023-06-01DOI: 10.1016/j.esci.2023.100114
Tianzhen Jian , Wenqing Ma , Caixia Xu , Hong Liu , John Wang
{"title":"Intermetallic-driven highly reversible electrocatalysis in Li–CO2 battery over nanoporous Ni3Al/Ni heterostructure","authors":"Tianzhen Jian , Wenqing Ma , Caixia Xu , Hong Liu , John Wang","doi":"10.1016/j.esci.2023.100114","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100114","url":null,"abstract":"<div><p>Li–CO<sub>2</sub> batteries, which integrate CO<sub>2</sub> utilization and electrochemical energy storage, offer the prospect of utilizing a greenhouse gas and providing an alternative to the well-established lithium-ion batteries. However, they still suffer from rather limited reversibility, low energy efficiency, and sluggish CO<sub>2</sub> redox reaction kinetics. To address these key issues, a nanoporous Ni<sub>3</sub>Al intermetallic/Ni heterojunction (NP–Ni<sub>3</sub>Al/Ni) is purposely engineered here via an alloying–etching protocol, whereby the unique interactions between Al and Ni in Ni<sub>3</sub>Al endow NP-Ni<sub>3</sub>Al/Ni with optimum reactant/product adsorption and thus unique catalytic performance for the CO<sub>2</sub> redox reaction. Furthermore, the nanoporous spongy structure benefits mass transport as well as discharge product storage and enables a rich multiphase reaction interface. <em>In situ</em> Raman studies and theoretical simulations reveal that both CO<sub>2</sub> reduction and the co-decomposition of Li<sub>2</sub>CO<sub>3</sub> and C are distinctly promoted by NP-Ni<sub>3</sub>Al/Ni, thereby greatly improving catalytic activity and stability. NP-Ni<sub>3</sub>Al/Ni offers promising application potential in Li–CO<sub>2</sub> batteries, with its scalable fabrication, low production cost, and superior catalytic performance.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"3 3","pages":"Article 100114"},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49883645","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
eSciencePub Date : 2023-06-01DOI: 10.1016/j.esci.2023.100113
Chengbo Wang , Yiting Jiang , Hanyu Xu , Nanlong Zheng , Guangsheng Bai , Yanxin Zha , Hao Qi , Zuqiang Bian , Xiaowei Zhan , Zhiwei Liu
{"title":"Enhancing performance of tin-based perovskite solar cells via fused-ring electron acceptor","authors":"Chengbo Wang , Yiting Jiang , Hanyu Xu , Nanlong Zheng , Guangsheng Bai , Yanxin Zha , Hao Qi , Zuqiang Bian , Xiaowei Zhan , Zhiwei Liu","doi":"10.1016/j.esci.2023.100113","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100113","url":null,"abstract":"<div><p>The performance of tin-based perovskite solar cells has been substantially hampered by voltage loss caused by energy level mismatch, charge recombination, energetic disorder, and other issues. Here, a fused-ring electron acceptor based on indacenodithiophene (IDIC) was for the first time introduced as a transition layer between a tin-based perovskite layer and a C<sub>60</sub> electron transport layer, leading to better matched energy levels in the device. In addition, coordination interactions between IDIC and perovskite improved the latter's crystallinity. The introduction of IDIC raised the power conversion efficiency from 8.98% to 11.5% and improved the device's stability. The decomposition mechanism of tin-based perovskite was also revealed by detecting the optical properties of perovskite microdomains through innovative integration of confocal laser scanning microscopy and photoluminescence spectroscopy.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"3 3","pages":"Article 100113"},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49883646","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
eSciencePub Date : 2023-06-01DOI: 10.1016/j.esci.2023.100121
Xue-Ting Li , Jia Chou , Yu-Hui Zhu , Wen-Peng Wang , Sen Xin , Yu-Guo Guo
{"title":"Hydrogen isotope effects: A new path to high-energy aqueous rechargeable Li/Na-ion batteries","authors":"Xue-Ting Li , Jia Chou , Yu-Hui Zhu , Wen-Peng Wang , Sen Xin , Yu-Guo Guo","doi":"10.1016/j.esci.2023.100121","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100121","url":null,"abstract":"<div><p>Aqueous rechargeable Li/Na-ion batteries have shown promise for sustainable large-scale energy storage due to their safety, low cost, and environmental benignity. However, practical applications of aqueous batteries are plagued by water's intrinsically narrow electrochemical stability window, which results in low energy density. In this perspective article, we review several strategies to broaden the electrochemical window of aqueous electrolytes and realize high-energy aqueous batteries. Specifically, we highlight our recent findings on stabilizing aqueous Li storage electrochemistry using a deuterium dioxide-based aqueous electrolyte, which shows significant hydrogen isotope effects that trigger a wider electrochemical window and inhibit detrimental parasitic processes.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"3 3","pages":"Article 100121"},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49884201","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
eSciencePub Date : 2023-06-01DOI: 10.1016/j.esci.2023.100119
Dan Wang , Junjun Mao , Chenchen Zhang , Jiawei Zhang , Junshan Li , Ying Zhang , Yongfa Zhu
{"title":"Modulating microenvironments to enhance CO2 electroreduction performance","authors":"Dan Wang , Junjun Mao , Chenchen Zhang , Jiawei Zhang , Junshan Li , Ying Zhang , Yongfa Zhu","doi":"10.1016/j.esci.2023.100119","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100119","url":null,"abstract":"<div><p>Microenvironments of the catalytic center, which play a vital role in adjusting electrocatalytic CO<sub>2</sub> reduction reaction (ECO<sub>2</sub>RR) activity, have received increasing attention during the past few years. However, controllable microenvironment construction and the effects of multi-microenvironment variations for improving ECO<sub>2</sub>RR performance remain unclear. Herein, we summarize the representative strategies for tuning the catalyst and local microenvironments to enhance ECO<sub>2</sub>RR selectivity and activity. The multifactor synergetic effects of microenvironment regulation for enhancing CO<sub>2</sub> accessibility, stabilizing key intermediates, and improving the performance of ECO<sub>2</sub>RR catalysts are discussed in detail, as well as perspectives on the challenges when investigating ECO<sub>2</sub>RR microenvironments. We anticipate that the discussions in this review will inspire further research in microenvironment engineering to accelerate the development of the ECO<sub>2</sub>RR for practical application.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":"3 3","pages":"Article 100119"},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49884202","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}