Hefeng Wang, Zixiao Li, Zhengwei Cai, Chaoxin Yang, Shengjun Sun, Xiaoyan Wang, Min Zhang, Yue Meng, Dongdong Zheng, Asmaa Farouk, Mohamed S. Hamdy, Xuping Sun, Bo Tang
{"title":"Ir nanoparticles decorated NiFe metal-organic framework as highly efficient and stable heterostructural electrocatalysts for overall seawater splitting","authors":"Hefeng Wang, Zixiao Li, Zhengwei Cai, Chaoxin Yang, Shengjun Sun, Xiaoyan Wang, Min Zhang, Yue Meng, Dongdong Zheng, Asmaa Farouk, Mohamed S. Hamdy, Xuping Sun, Bo Tang","doi":"10.1039/d4ta06515h","DOIUrl":"https://doi.org/10.1039/d4ta06515h","url":null,"abstract":"Developing a bifunctional electrocatalyst for overall seawater splitting is crucial for advancing sustainable hydrogen (H2) production. However, at industrial current densities, anodic chlorine chemical corrosion and cathodic sluggish hydrogen evolution kinetics will seriously hinder the system of seawater-to-H2. Herein, we present a heterojunction electrocatalyst synthesized via hydrothermal methods to create ultrathin NiFe-MOF nanosheets on nickel foam, followed by the deposition of Ir nanoparticles through a redox strategy (Ir@NiFe-MOF/NF). Ir@NiFe-MOF/NF demonstrates exceptional alkaline seawater oxidation and reduction properties, achieving a current density of 1000 mA cm−2 with overpotentials of 445 and 233 mV. Additionally, it requires only a voltage of 2.11 V to drive 250 mA cm−2 in a membrane electrode device and operates stably for 400 hours in alkaline seawater, surpassing other recently reported bifunctional electrocatalysts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580720","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"A Solid-State Electrolyte Based on Electrochemical Active LiMn2O4 for Lithium Metal Batteries","authors":"Jingzhen Du, Zhichao Chen, Bohao Peng, Zewen Sun, Wenzhuo Wu, Qi Zhou, Xia Shuang, Lili Liu, Lijun Fu, Yuhui Chen, Tao Wang, Yuping Wu","doi":"10.1039/d4ta05743k","DOIUrl":"https://doi.org/10.1039/d4ta05743k","url":null,"abstract":"The key to the practical application of lithium metal batteries (LMBs) lies in developing solid state electrolytes (SSEs) that are simple to prepare and exhibit excellent performance. In this work, commercial and cheap cathode material LiMn<small><sub>2</sub></small>O<small><sub>4</sub></small> (LMO) is used as an SSE and mixed with poly(vinylidene difluoride) (PVDF) to create SSEs aimed at improving interfacial stability and electronic insulation. The LMO-3 SSE, containing 30 wt.% LMO, demonstrates high ionic conductivity (5.17 × 10<small><sup>-4</sup></small> S cm<small><sup>-1</sup></small> at 35 °C), low electronic conductivity (< 10<small><sup>−9</sup></small> S cm<small><sup>−1</sup></small>), and good interfacial contact and stability with both the lithium metal anode and LiFePO<small><sub>4</sub></small> (LFP) cathode. The Li||LFP cell with LMO-3 exhibits good cycling stability at a current density of 0.5 C (200 cycles, maintaining a discharge specific capacity of 147.7 mAh g<small><sup>-1</sup></small>, with a capacity retention rate of 96.0% and a coulombic efficiency of 99.8%). This study provides a direction for the application of LMO in high-performance SSEs and LMBs, paving another economic route to the commercialization of solid-state lithium metal batteries.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
John D. Langhout, Elizabeth Gager, Talianna Ulloa, Shane Shepard, Juan C. Nino, Megan M. Butala
{"title":"Isovalent substitution modulates average and short-range structure in disordered rocksalt oxides","authors":"John D. Langhout, Elizabeth Gager, Talianna Ulloa, Shane Shepard, Juan C. Nino, Megan M. Butala","doi":"10.1039/d4ta05971a","DOIUrl":"https://doi.org/10.1039/d4ta05971a","url":null,"abstract":"Li-excess disordered rocksalt oxides are promising candidate materials for high-energy density Li-ion battery cathodes. Their disordered cation sublattice provides opportunity to design compositions that balance performance and sustainability, especially enabling the use of abundant and inexpensive elements. However, relationships between composition, short-range cation ordering, and their effects on performance are not well-understood. Here, we use a compositional series of the form Li<small><sub>1.2</sub></small>Mn<small><sub>0.4</sub></small>Ti<small><sub>0.4−<em>x</em></sub></small>Zr<small><sub><em>x</em></sub></small>O<small><sub>2</sub></small>, in which Ti<small><sup>4+</sup></small> is gradually replaced with Zr<small><sup>4+</sup></small>, to study the effect of Zr content on average- and short-range structure using synchrotron X-ray diffraction and pair distribution function analysis. We report the coexistence of multiple modes of short-range order, which have a major impact on battery capacity. However, the effects of Zr on degree of short-range ordering, lattice parameter, and chemical segregation also influence battery capacity, reflecting the complex dependencies of composition on structure across length scales in these disordered materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580165","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Ultrahigh cycling stability and wide infrared modulation of electrochromic devices based on electrodeposited triphenylamine cross-linked polyaniline derivatives","authors":"Yulin Liu, Hengzhi Zhang, Shengwei Tang, Rongzong Zheng, Chunyang Jia","doi":"10.1039/d4ta05607h","DOIUrl":"https://doi.org/10.1039/d4ta05607h","url":null,"abstract":"Reflective electrochromic devices (RECDs) based on polyaniline (PANI) have garnered significant attention due to their broad-band modulation capabilities. However, the inherent unstable molecular structure of PANI remains a major challenge, affecting both its cycling stability and modulation range. To address this issue, triphenylamine and <em>m</em>-phenylenediamine were introduced to prepare cross-linked PANI (CPANI) electrochromic thin films <em>via</em> a straightforward electrodeposition process in this paper. The thermal-infrared emissivity modulation range of the CPANI-based RECD (C-RECD) achieved great improvement in the atmospheric windows of 3–5 and 8–14 μm, with a maximum emissivity modulation range of 0.5 and 0.7, respectively. Remarkably, the C-RECD exhibits exceptional cycling stability, enduring up to 10 000 cycles, while maintaining a 70% average emissivity modulation range after cycling. The excellent modulation capability and cycling stability of the C-RECD break the record of the PANI-based RECDs. The theoretical calculations, <em>in situ</em> Raman spectroscopy, and emittance spectra were examined to gain insights into the crosslinking enhancement mechanism. Its distinctive cross-linked structure promotes electron delocalization within the PANI chain, which facilitates an increase in the number of polarons and hinders the formation of local quinoid over-oxidation units, thus effectively improving its emissivity modulation capability and cycling stability. The thermal-infrared images demonstrate the apparent temperature management effects at 7.2 °C and 13.3 °C when the C-RECD is integrated with human skin and a hot plate. This work provides promising opportunities for the production of long-term stable anti-reconnaissance and thermal management devices based on PANI-based RECDs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580166","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Novel Polar Oxides with Exceptional Pyroelectric Performance: Doping-Induced Polar Transition in Ba6Pb3.2(PO4)6Cl2","authors":"Duo Zhang, Ruijin Sun, Zhaolong Liu, Haodong Li, Munan Hao, Yuxin Ma, Ke Ma, Dezhong Meng, Zhiyuan Zheng, Yibo Xu, Xu Chen, Qiu Fang, Xuefeng Wang, Linjie Dai, Changchun Zhao, Shifeng Jin","doi":"10.1039/d4ta06308b","DOIUrl":"https://doi.org/10.1039/d4ta06308b","url":null,"abstract":"Among existing pyroelectric materials, inorganic polar oxides exhibit large pyroelectric coe-fficients. However, their pyroelectric performance is severely limited by the high dielectric constants due to the inverse relationship between pyroelectric figures of merit (FOMs) and dielectric constants. On the other hand, organic pyroelectric materials, while having lower dielectric constants and losses, suffer from poor stability, which greatly restricts their applica-tion. Regarding the above issues, we present a novel class of polar oxides, Ba6Pb3.2(PO4)6Cl2 (BPPC) and Ba6(Bi0.5Na0.5)4(PO4)6Cl2 (BBNPC), derived from a previously unreported tran-sformation of non-polar apatite structures. These materials exhibit exceptionally low dielectric constants (~10) and losses (~0.002), combined with high stability. Notably, BPPC demonstr-ates outstanding pyroelectric performance, with a pyroelectric coefficient of 110 μC/m2/K. The pyroelectric figures of merit (FOMs) for BPPC (room-temperature Fv = 0.7 m2/C, FD = 17.0×10-5 Pa1/2, FE = 5.12 ×10-11 m3/J) surpass those of most existing inorganic pyroelectrics and approach the performance of leading organic materials. This pioneering doping strategy, leverageing size differentiated atomic substitution to induce spontaneous polarization, opens new avenues for designing high-performance polar oxides with potential applications in ferro-electric, piezoelectric, and photonic technologies. Our findings significantly expand the scope of polar function-al materials beyond traditional perovskite-type oxides.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574380","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Unexpected Anion Segregation Enabling High Conductivity in Argyrodite Li6–xPS5–xClBrx Solid Electrolytes","authors":"Seho Yi, Taegon Jeon, Gyeong Ho Cha, Young-Kyu Han, Sung Chul Jung","doi":"10.1039/d4ta06120a","DOIUrl":"https://doi.org/10.1039/d4ta06120a","url":null,"abstract":"Site disorder between S and Cl anions at Wyckoff 4a and 4d sites is a key structural feature of the argyrodite Li6PS5Cl solid electrolyte in all-solid-state batteries. This first-principles study on the Li5.75PS4.75ClBr0.25 system is the first to report that S/Cl/Br anion disorder leads to an unexpected segregation of two anion sublattice domains, one composed of S anions and the other composed of Cl/Br anions. Increasing the degree of anion disorder enhances the stability of Li5.75PS4.75ClBr0.25, resulting in the formation of the most stable structure with anion segregation when the highest degree of anion disorder is reached. The anion segregation causes a greater distribution of Li ions in the S domain than in the Cl/Br domain, which greatly reduces the repulsion between S2– ions compared to the repulsion between Cl–/Br– ions and effectively stabilizes Li5.75PS4.75ClBr0.25. Li ions in the S domain move with difficulty due to the strong Li−S bonds, whereas Li ions in the Cl/Br domain can move relatively freely due to the weak Li−Cl (Li−Br) bonds, resulting in a high conductivity of 10.1 mS cm−1. This study suggests that domain-dependent Li migration due to anion segregation is the fundamental ion transport mechanism in Li6–xPS5–xClBrx and offers a new perspective for understanding superionic conductivity in Li6PS5Cl-based argyrodite solid electrolytes.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574381","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Seung Uk Son, Yoon Kee Kim, Sang Lim Park, Jong Doo Lee
{"title":"Hexagonal CeO2 nanoplate@Au catalysts for the selective oxidation of 1,3-propanediol to a polymer platform, 3-hydroxypropionic acid at room temperature","authors":"Seung Uk Son, Yoon Kee Kim, Sang Lim Park, Jong Doo Lee","doi":"10.1039/d4ta06419d","DOIUrl":"https://doi.org/10.1039/d4ta06419d","url":null,"abstract":"Hexagonal CeO2 plates (H-CeO2) were prepared through template synthesis using a 2D hexagonal microporous organic polymer (H-MOP). After loading Au species onto H-CeO2, the resulting H-CeO2@Au was studied as a heterogeneous catalyst for the selective oxidation of 1,3-propanediol into an important polymer platform, 3-hydroxypropionic acid (3HP). The optimized catalyst, H-CeO2@Au-2, achieved a 91% yield of 3HP at room temperature under ambient 1 atm O2 and demonstrated recyclability over five successive runs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580170","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ramees Jebin P, Andrew Simon George, Rakesh K. Mishra, Jubi John, Suraj Soman
{"title":"Enhanced indoor photovoltaic efficiency of 40% in dye-sensitized solar cells using cocktail starburst triphenylamine dyes and dual species copper electrolyte","authors":"Ramees Jebin P, Andrew Simon George, Rakesh K. Mishra, Jubi John, Suraj Soman","doi":"10.1039/d4ta05513f","DOIUrl":"https://doi.org/10.1039/d4ta05513f","url":null,"abstract":"Recombination is the most critical process that controls the photovoltaic performance in dye-sensitized solar cells (DSCs). Herein, we successfully introduced a new triphenylamine-based starburst photosensitizer, RJ-C6 [3-(4-(bis(4-((2,4-bis(hexyloxy)phenyl)ethynyl)phenyl)amino)phenyl)-2-cyanoacrylic acid] grafted with extended alkyl groups and phenylethynyl bridges capable of arresting recombination more effectively and realizing enhanced light harvesting through improved conjugation and rigidity. Using a cocktail mixture of RJ-C6 with XY1b dye and asymmetric dual species copper (II/I) electrolyte, we realized an efficiency of 10.40% under standard AM 1.5G, 100 mW/cm2 irradiation. Strikingly, the same co-sensitized devices exhibited a panchromatic absorption overlapping the entire fluorescent light spectra, delivering an efficiency of 35% under 100 lux, 37% under 1000 lux and a record PCE of 40% under 4000 lux fluorescent light illumination, taking DSC one step closer to being used as an attractive successor for indoor photovoltaic applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580264","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yang Song, Haidong Zhong, Tingting Hu, Qizhi Chen, Lei Shi, Jun Du, Changyuan Tao, Qian Zhang
{"title":"Dually Encapsulated LiMn0.6Fe0.4PO4 Architecture with MXene and Amorphous Carbon to Achieve High-performance and Ultra-stable Lithium Battery","authors":"Yang Song, Haidong Zhong, Tingting Hu, Qizhi Chen, Lei Shi, Jun Du, Changyuan Tao, Qian Zhang","doi":"10.1039/d4ta06323f","DOIUrl":"https://doi.org/10.1039/d4ta06323f","url":null,"abstract":"LiMnxFe1-xPO4 (LMFP) materials, with their high energy density and excellent cycle stability, are promising cathode materials for electric vehicles and other high-energy-density applications. However, the low lithium-ion diffusion coefficient and poor electronic conductivity limit the further development of LMFP. In this study, we designed a strategy involving electrostatic self-assembly and in-situ graphitization to fabricate a dense LMFP@MXene@C structure with dual encapsulation of LMFP (LiMn0.6Fe0.4PO4). Owing to its high degree of graphitization, large surface area, excellent Li-ion directional transport, and dense dual encapsulation structure, the fabricated LMFP@MXene@C cathode exhibits a considerable reversible capacity (153.58 mAh/g after 100 cycles at 1 C) with outstanding rate performance and stability (maintaining 91.26% of its capacity after 1200 cycles at 5 C). According to the detailed TEM, in-situ XRD techniques, and system dynamics and structural stability assessments analysis, the superior electrochemical stability and Li+ transport can be attributed to the network structure formed by 2D MXene layered channels and amorphous C layers. This structure facilitates the rapid electron and ion transfer, effectively providing volumetric buffering and structural protection. The dually encapsulated strategy offers a feasible approach for the preparation of exceptional electrochemical cathode materials.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574377","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ting Su, Wenjun Liu, Hao Xu, Huilong Chen, Kin Long Wong, Wanru Zhang, Qingting Su, Tongxin Wang, Shanlei Xu, Xingting Liu, Weiwei Lv, Renyong Geng, Jun Yin, Xin Song
{"title":"Self-Assembling Hole-Transport Material Incorporating Biphosphonic Acid for Dual-Defect Passivation in NiOx-Based Perovskite Solar Cells","authors":"Ting Su, Wenjun Liu, Hao Xu, Huilong Chen, Kin Long Wong, Wanru Zhang, Qingting Su, Tongxin Wang, Shanlei Xu, Xingting Liu, Weiwei Lv, Renyong Geng, Jun Yin, Xin Song","doi":"10.1039/d4ta05776g","DOIUrl":"https://doi.org/10.1039/d4ta05776g","url":null,"abstract":"The efficiency and stability of nickel oxide (NiOx)-based perovskite solar cells (PSCs) are critically hindered by defects and suboptimal charge transfer at the interface between perovskite crystals and the NiOx layer. In this study, we introduce a self-assembled hole transport material, D-3PACz, featuring bisphosphonic acid anchoring groups, to address these challenges. D-3PACz is proved to be effective in improving the surface properties of nickel oxide, optimizing the energy level alignment, and enhancing hole extraction capability. Meanwhile, the robust interaction between phosphonic acid and the perovskite layer enables D-3PACz to effectively direct the growth of perovskite crystals. These findings result in devices exhibiting reduced non-radiative recombination losses, lower defect-state densities, and enhanced hole extraction performance, culminating in a comprehensive improvement in device parameters. Excitingly, the D-3PACz based devices obtain a champion PCE of 23.8% with elevated stability. Our work presents the superiority of the proposed D-3PACz material for efficient and stable PSCs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574378","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}