Journal of Materials Chemistry A最新文献

Discovering Virtual Na-based Argyrodites as Solid-State Electrolytes Using DFT, AIMD, and Machine Learning Techniques 利用 DFT、AIMD 和机器学习技术发现作为固态电解质的虚拟 Na 基 Argyrodites

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-11-18 DOI: 10.1039/d4ta06927g

Kee-Sun Sohn, Byung Do Lee, Deepak S. Gavali, Heejeong Kim, Seonghwan Kim, Min Young Cho, Kyunglim Pyo, Young-Kook Lee, Woon Bae Park

{"title":"Discovering Virtual Na-based Argyrodites as Solid-State Electrolytes Using DFT, AIMD, and Machine Learning Techniques","authors":"Kee-Sun Sohn, Byung Do Lee, Deepak S. Gavali, Heejeong Kim, Seonghwan Kim, Min Young Cho, Kyunglim Pyo, Young-Kook Lee, Woon Bae Park","doi":"10.1039/d4ta06927g","DOIUrl":"https://doi.org/10.1039/d4ta06927g","url":null,"abstract":"In surveying an extensive library of 4,375 hypothetical Na-based Argyrodites, we underscore the value of computational screening, noting that no Na-based Argyrodite solid-state electrolyte has been successfully synthesized. We introduce a robust approach using density functional theory (DFT) calculations to identify thermodynamically and electrochemically stable candidates. By evaluating energy above the hull (Eh), formation energy (Ef), band gap (Eg), and electrochemical stability window (Vw), we narrow the set to 15 compounds via a 4-dimensional Pareto frontier. Competing materials for Eh and Vw calculations are sourced from the Materials Project, ICSD, and Google DeepMind. Connectivity-optimized graph networks validate the reliability of our calculations. Ab-initio molecular dynamics (AIMD) calculations assess the room-temperature sodium ion conductivity (σRT) of the 15 selected entries, ultimately identifying the top 5 with promising σRT. This discovery of multi-compositional virtual Argyrodites advances the challenge of synthesizing Na-based Argyrodites.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"22 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665449","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}

引用次数: 0

Efficient Caustic and Hydrogen Production Using a Pressurized Flow-Through Cathode 利用加压穿流阴极高效生产苛性碱和氢气

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-11-18 DOI: 10.1039/d4ta04680c

Fan Yang, Minhao Xiao, Sangsuk Lee, Javier Alan Quezada Rentería, Xinyi Wang, Minju Cha, Anya Rose Dickinson-Cove, Sungsoon Kim, Guy Z. Ramon, Gaurav Sant, Eric M. V. Hoek, David Jassby, Igor M De Rosa

{"title":"Efficient Caustic and Hydrogen Production Using a Pressurized Flow-Through Cathode","authors":"Fan Yang, Minhao Xiao, Sangsuk Lee, Javier Alan Quezada Rentería, Xinyi Wang, Minju Cha, Anya Rose Dickinson-Cove, Sungsoon Kim, Guy Z. Ramon, Gaurav Sant, Eric M. V. Hoek, David Jassby, Igor M De Rosa","doi":"10.1039/d4ta04680c","DOIUrl":"https://doi.org/10.1039/d4ta04680c","url":null,"abstract":"The emerging process of CO2 capture and sequestration will likely require large volumes of caustic. The fossil fuel demand and carbon footprint of transporting liquid caustic is self-defeating, and hence, there is a need for energy-efficient, on-site caustic production for carbon capture projects. Caustic production is dominated by the well-established “chlor-alkali” processes. This process requires highly concentrated (~25 wt.%) and pure (>99.5 wt.%) NaCl feed brines, uses high-cost ion-exchange membranes and high operating temperatures (90 C), and generates a highly-concentrated (>33%) caustic stream that can be further concentrated using thermal evaporation. This highly concentrated caustic is then shipped to customers, where it is typically diluted to the required level. We have developed a flow-through membrane/cathode electrolysis process that produces a caustic solution (pH 10.22-12.26) at a specific energy consumption (SEC) of 1.71 kWhe/kg NaOH at room temperature using a 3.5% NaCl solution as feed, while achieving pure H2 generation without the use of ion exchange membranes. We demonstrate that the SEC is strongly dependent on the flow rate through the cathode, reaching a minimum at a high rate of 1,200 L/m2/hr. Electrochemical impedance spectroscopy, confocal microscopy, and finite element modeling show that the SEC is lowered through a combination of enhanced mass transport (of H+ and OH- ions) to and from the cathode surface and H2 gas stripping, both facilitated by the high flow rates. This technology offers the opportunity for the on-site production of dilute caustic streams (potentially from softened seawater) at a significantly reduced energy cost (compared to conventional chlor-alkali processes that consume >2.1 kWhe/kg NaOH).","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"6 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665446","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}

引用次数: 0

Alloying induced superionic β-phase formation in Mg3Sb2 based Zintl compounds 在 Mg3Sb2 基 Zintl 化合物中形成合金诱导的超离子 β 相

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-11-18 DOI: 10.1039/d4ta06173j

Nagendra Singh Chauhan, Takao Mori

{"title":"Alloying induced superionic β-phase formation in Mg3Sb2 based Zintl compounds","authors":"Nagendra Singh Chauhan, Takao Mori","doi":"10.1039/d4ta06173j","DOIUrl":"https://doi.org/10.1039/d4ta06173j","url":null,"abstract":"The off-centering phenomenon manifests as locally distorted configurations with broken symmetry in a crystal structure due to the displacement of constituent atoms from their ideal coordination centers within the lattice. In contrast to the anticipated formation of anionic solid solutions of Mg3(Sb1−x−yBixGey)2, herein we report β-Mg3(Sb, Bi)2 based superionic phase formation (space group – Ia<img alt=\"[3 with combining macron]\" border=\"0\" src=\"https://www.rsc.org/images/entities/char_0033_0304.gif\"/>, 206) with off-centering of the dominant trigonal α-Mg3(Sb, Bi)2 phase and segregation of nanophase Mg3Ge upon equiatomic (Bi, Ge) alloying. The discordant nature of Ge is unveiled within the layered α-Mg3(Sb, Bi)2 structure and is assessed employing (3 + 1) dimensional superspace to reveal an off-centering (dz) along the z direction for the constituent atoms in the range of ±0–0.02 Å. The (Bi, Ge) alloying results in favourable tuning of the desired p-type conduction for attaining higher power factors by band engineering and synergistic reduction of lattice thermal conductivity. The stable superionic polymorph co-existing in an anionic solid solution of Mg3(Sb, Bi)2 provides a renewed basis for understanding the crystal structure and its transformation in CaAl2Si2-type Zintl compounds.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"18 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665394","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}

引用次数: 0

Enhancing photoactivity of defective g-C3N4 via self-polarization effect of tourmaline for CO2 reduction 通过电气石的自极化效应提高有缺陷 g-C3N4 的光活性，用于二氧化碳还原

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-11-18 DOI: 10.1039/d4ta06709f

Jiangpeng Wang, Chao Huang, Deng Liu, Huihui Peng, Qiong Luo, Dimin Yang, Xuelian Yu, Yingmo Hu

{"title":"Enhancing photoactivity of defective g-C3N4 via self-polarization effect of tourmaline for CO2 reduction","authors":"Jiangpeng Wang, Chao Huang, Deng Liu, Huihui Peng, Qiong Luo, Dimin Yang, Xuelian Yu, Yingmo Hu","doi":"10.1039/d4ta06709f","DOIUrl":"https://doi.org/10.1039/d4ta06709f","url":null,"abstract":"Graphite carbon nitride (g-C3N4) has been extensively studied as a non-metallic catalyst for photocatalytic reduction of CO2. However, its efficiency and selectivity in CO2 reduction still require further enhancement. In this study, we have incorporated the silicate mineral tourmaline, known for its spontaneous polarization properties, into g-C3N4 with nitrogen defects. The novel composite catalyst, named TM/CN(NH), was synthesized by a two-step method of high-temperature calcination. The optimal composite ratio of the sample (25TM/CN(NH)) can achieve a CO yield rate of 118.17 μmol g-1 h-1, which is 6.4 times that of the bulk g-C3N4(CN) and 2.9 times that of g-C3N4 containing N defects (CN(NH)). Our findings indicate that the self-polarization effect of tourmaline and the introduction of nitrogen vacancies can remarkably upgrade the photocatalytic efficiency of g-C3N4. On one hand, the nitrogen vacancies can broaden the light absorption range of g-C3N4, optimize its band gap structure, and improve its efficiency in utilizing light energy. On the other hand, the electric field generated by the self-polarization effect of tourmaline can enhance the migration of electrons in the lattice of g-C3N4, promote the migration and separation of electrons and holes, and thus increase the reduction efficiency of CO2 by g-C3N4. This research innovatively integrates cost-effective mineral materials into g-C3N4, significantly elevating the photocatalytic capabilities of g-C3N4. Furthermore, it paves the way for the rational design of abundant and inexpensive catalysts, aiming to achieve efficient photocatalytic carbon dioxide reduction.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"25 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665450","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}

引用次数: 0

Correction: MOF-derived CeO2 catalysts with Pr doping: engineering oxygen vacancies for improved CO2 conversion to dimethyl carbonate 更正：掺杂 Pr 的 MOF 衍生 CeO2 催化剂：利用氧空位工程改善二氧化碳到碳酸二甲酯的转化率

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-11-18 DOI: 10.1039/d4ta90220c

Jungseob So, Min Hye Jeong, Jungwon Yun, Byeong-Seon An, Seung-ik Kim, Geun-yeong Kim, Hyun-Tak Kim, Tae Sun Chang, Jin Hee Lee, Iljeong Heo, Jinjoo An, Young-Woo You, Minkyu Kim, Young Jin Kim

引用次数: 0

Synthesis of Nd3+-doped α-γ bismuth oxide homojunction nanoparticles: a smart multifunctional solar photocatalyst 掺杂 Nd3+ 的 α-γ 氧化铋同质纳米颗粒的合成：一种智能型多功能太阳能光催化剂

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-11-18 DOI: 10.1039/d4ta04637d

Aji Joseph, Ambili K. S., Anju John, Minjoong Yoon, Jesty Thomas

{"title":"Synthesis of Nd3+-doped α-γ bismuth oxide homojunction nanoparticles: a smart multifunctional solar photocatalyst","authors":"Aji Joseph, Ambili K. S., Anju John, Minjoong Yoon, Jesty Thomas","doi":"10.1039/d4ta04637d","DOIUrl":"https://doi.org/10.1039/d4ta04637d","url":null,"abstract":"Multifunctional Nd3+-doped α-γ bismuth oxide (Bi2O3) homojunction nanoparticles were successfully synthesized through metamorphosis from the α-β Bi2O3 homojunction via a low temperature solvothermal method. The structural and optical properties were thoroughly characterized by different methods. NIR reflectance spectroscopy revealed that 2 wt% Nd3+-doped Bi2O3 exhibited about 90% NIR reflectance. The CIE-L*a*b* 1976 colour analysis showed a b* value of 50.72, surpassing that of the commercially available yellow pigment Zircon Yellow, which has a b* value of 43.3. The transformation from α-β to α-γ Bi2O3 was controlled by dopant concentration, with the band gap decreasing as the Nd3+ content increases. The synthesized materials demonstrated efficient photocatalytic activity, degrading model pollutant methylene blue and the antibiotic ceftriaxone sodium under sunlight. This was investigated using UV-visible spectroscopy and LC-MS. The α-γ Bi2O3 homojunction presents a promising new direction for eco-friendly cool yellow pigments that degrade organic pollutants under sunlight showing upconversion luminescence and antibacterial activity.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"50 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665448","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}

引用次数: 0

A local Proton−Transport Promoter for Industrial CO2 Electroreduction to Multicarbon Products 用于工业二氧化碳电还原成多碳产品的本地质子传输促进剂

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-11-16 DOI: 10.1039/d4ta04672b

Haiyi Guo, Qi Huang, Di Li, Shiyu Dai, Kang Yang, Sheng Chen, Wei Ma, Qiang Li, Jingjing Duan

{"title":"A local Proton−Transport Promoter for Industrial CO2 Electroreduction to Multicarbon Products","authors":"Haiyi Guo, Qi Huang, Di Li, Shiyu Dai, Kang Yang, Sheng Chen, Wei Ma, Qiang Li, Jingjing Duan","doi":"10.1039/d4ta04672b","DOIUrl":"https://doi.org/10.1039/d4ta04672b","url":null,"abstract":"Industrial carbon dioxide electroreduction (eCO2RR) is of wide interests, also a great challenge to ensure sufficient and fast mass supply to achieve industrial-level current densities. Herein, a local proton-transport promoter has been developed by hybridizing Cu catalytic sites with proton hopping sites from dual-conductive polymers to tackle the mass-diffusion limit. The Cu/Polypyrrole exhibits extraordinary eCO2RR to C2+ performance with a high FEC2+ of 80.0% under an industrial current density of 700 mA/cm-2. Experimentally and theoretically, it is found protons transfer via a Grotthuss mechanism, whose conductivity is determined by the hydrogen bond formation and breakage (“-HN1---H N2H-” to “-HN1 H---N2H-”) at the hopping site from the dual-conductive Polypyrrole, rather than diffusion coefficient of the proton source and hydrous/anhydrous protons. Significantly, the advantageous proton transport of Cu/PPy is further confirmed by an in situ scanning electrochemical microscope testing, according to the proton change in the diffusion layer and local catalytic sites.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"98 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642966","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}

引用次数: 0

Root-Cause Analyses for 3D Intermolecular Packing Network Formation in Central Unit Extended Small Molecular Acceptors 中心单元扩展小分子受体分子间三维堆积网络形成的根源分析

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-11-15 DOI: 10.1039/d4ta07485h

Jiaxin Guo, Xiangjian Cao, Zheng Xu, Tengfei He, Xingqi Bi, Zhaoyang Yao, Yaxiao Guo, Guankui Long, Chenxi Li, Xiangjian Wan, Yongsheng Chen

{"title":"Root-Cause Analyses for 3D Intermolecular Packing Network Formation in Central Unit Extended Small Molecular Acceptors","authors":"Jiaxin Guo, Xiangjian Cao, Zheng Xu, Tengfei He, Xingqi Bi, Zhaoyang Yao, Yaxiao Guo, Guankui Long, Chenxi Li, Xiangjian Wan, Yongsheng Chen","doi":"10.1039/d4ta07485h","DOIUrl":"https://doi.org/10.1039/d4ta07485h","url":null,"abstract":"The enhanced three-dimensional (3D) intermolecular packing network in central unit extended small molecular acceptors (SMAs) has boosted the performance of organic solar cells (OSCs) significantly by improving the inner exciton/charge photodynamic. However, the structural profiles that determine the formation of efficient 3D packing network are still shrouded in mystery. Herein, a series of SMAs (CH1, CH2, CH3, CH20 and CH8F) with/without central conjugation extension and substitutions are systematically investigated at both single-molecule and aggregate levels. Notably, by examining the evolution of packing networks and modes from CH1 to CH8F, the determining role of central unit extension and halogenation in constructing an enhanced 3D intermolecular packing network is revealed for the first time. Additionally, binary OSCs of CH8F, which combine central extension with fluorination achieve a first-class power conversion efficiency (PCE) of 19.02%, markedly outperforming its counterparts. These root-cause analyses unveil the essential structural elements for forming superior 3D packing networks and will further boost rational design of SMAs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"21 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637845","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}

引用次数: 0

Enhanced Electrochemical Performance of NiSbS/NiSb/NiS Nanocomposites Anchored on Graphite Nanosheets for Sodium-Ion Battery Applications 锚定在钠离子电池应用石墨纳米片上的 NiSbS/NiS/NiS 纳米复合材料的增强电化学性能

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-11-15 DOI: 10.1039/d4ta07323a

Shandong Huang, Dong Feng, Yuanzhi Zhu, Yihong Ding, Delong Xie, Yi Mei, Zeng tianbiao

{"title":"Enhanced Electrochemical Performance of NiSbS/NiSb/NiS Nanocomposites Anchored on Graphite Nanosheets for Sodium-Ion Battery Applications","authors":"Shandong Huang, Dong Feng, Yuanzhi Zhu, Yihong Ding, Delong Xie, Yi Mei, Zeng tianbiao","doi":"10.1039/d4ta07323a","DOIUrl":"https://doi.org/10.1039/d4ta07323a","url":null,"abstract":"In the realm of scalable fabrication of anodes through ball-milling, ensuring high electrochemical performance and robust cycling stability anodes for sodium-ion batteries is paramount but presents a formidable hurdle. In pursuit of these goals, a distinctive hybrid composite distinguished by its intricate multiphase composition have devised. This entails the integration of innovative NiSbS/NiSb/NiS nanomaterials onto exfoliated graphite nanosheets (Ni-Sb-S/GN) via a straightforward technique. Analyses indicates the interplay between graphite nanosheets and the hybrid Ni-Sb-S, in conjunction with the discharge byproducts of Na2S, substantially augment the stability and Na-ion diffusion kinetics of the Ni-Sb-S/GN anode. The novel Ni-Sb-S/GN exhibits markedly superior electrochemical performance in comparison to its Ni-Sb-S counterpart. Specifically, Ni-Sb-S/GN achieves a reversible capacity of 238.7 mAh g-1 at 0.2 A g-1 post 300 cycles, remains notable capacities of 200 mAh g-1 after 1000 cycles under 1 A g-1, respectively, translating to high capacity retention rates of 83.8% from the 2nd cycle. This contribution presents a novel avenue for the exploitation of advanced multiphase anodes exhibiting superior capacity, rate capability, and cycling durability.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"21 1","pages":""},"PeriodicalIF":11.9,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637573","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}

引用次数: 0

Inverse analysis-guided development of acid-tolerant nanoporous high-entropy alloy catalysts for enhanced water-splitting performance 以逆向分析为指导开发耐酸性纳米多孔高熵合金催化剂，提高水分离性能

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-11-15 DOI: 10.1039/d4ta05756b

Saikat Bolar, Chunyu Yuan, Samuel Jeong, Yoshikazu Ito, Takeshi Fujita

引用次数: 0