{"title":"Bi-S Bond Mediated Direct Z-Scheme BiOCl/Cu2SnS3 Heterostructure for Efficient Photocatalytic Hydrogen Generation.","authors":"Dipendu Sarkar, Maitrayee Biswas, Swarup Ghosh, Joydeep Chowdhury, Biswarup Satpati, Srabanti Ghosh","doi":"10.1002/cssc.202402655","DOIUrl":"https://doi.org/10.1002/cssc.202402655","url":null,"abstract":"<p><p>The advancement of photocatalytic technology for solar-driven hydrogen (H2) production remains hindered by several challenges in developing efficient photocatalysts. A key issue is the rapid recombination of charge carriers, which significantly limits the light-harvesting ability of materials like BiOCl and Cu2SnS3 quantum dots (CTS QDs), despite the faster charge mobility and quantum confinement effect, respectively. Herein, a BiOCl/CTS (BCTS) heterostructure was synthesized by loading CTS QDs onto BiOCl 2D nanosheets (NSs), that demonstrated excellent photocatalytic activity under visible light irradiation. The improved hydrogen generation rate (HGR) was primarily due to an interfacial Bi-S bond formation, which facilitates the creation of direct Z-scheme heterojunction and an internal electric field at the interface, promoting efficient charge transfer between BiOCl and CTS. Moreover, due to the amalgamation of Bi-S bond formation and interfacial electric field, the optimized BCTS-5% heterostructure exhibited a high HGR of 8.27 mmol·g⁻¹·h⁻¹, and an apparent quantum yield (AQY) of 61%, ~ 4 times higher than pristine BiOCl. First-principles density functional theory (DFT) calculations further revealed the presence of a Bi-S bond with a bond length of ~2.85 Å and a minimal work function of 2.37 eV for the heterostructure, both of which are critical for enhancing H2 generation efficiency.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402655"},"PeriodicalIF":7.5,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143045100","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"In-Situ Construction of LiCl-Rich Artificial Solid Electrolyte Interphase for High-Performance Lithium Metal Anode.","authors":"Zhen Chen, Xi Wang, Shengjie Qian, Hai-Peng Liang, Minghua Chen, Zexiang Shen","doi":"10.1002/cssc.202402638","DOIUrl":"https://doi.org/10.1002/cssc.202402638","url":null,"abstract":"<p><p>In the pursuit of high-energy-density lithium metal batteries (LMBs), the development of stable solid electrolyte interphase (SEI) is critical to address issues such as lithium dendrite growth and low Coulombic efficiency. Herein, we propose a facile strategy for the in-situ fabrication of a LiCl-rich artificial SEI layer on Li surfaces through reaction of MoCl5 with Li (Li@MoCl5). The resulting artificial SEI significantly enhances the uniformity of Li deposition, effectively suppresses dendrite formation, and improves electrochemical performance. As a result, Li@MoCl5 symmetric cells demonstrate remarkable stability, achieving continuous cycling of 4200 h under a high current density of 10 mA cm-2 with an areal capacity of 1 mAh cm-2. Full-cells employing Li@MoCl5 exhibit superior cycling stability and rate capability, even at high cathode loading (17 mg cm-2). These results highlight the potential of this interface engineering strategy for advanced practical application of LMBs.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402638"},"PeriodicalIF":7.5,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143045104","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Inulin Dehydration to 5-HMF in Deep Eutectic Solvents Catalyzed by Acidic Ionic Liquids Under Mild Conditions.","authors":"Salvatore Marullo, Giovanna Raia, Josh J Bailey, H Q Nimal Gunaratne, Francesca D'Anna","doi":"10.1002/cssc.202402522","DOIUrl":"https://doi.org/10.1002/cssc.202402522","url":null,"abstract":"<p><p>Valorization of carbohydrate-rich biomass by conversion into industrially relevant products is at the forefront of research in sustainable chemistry. In this work, we studied the inulin conversion into 5-hydroxymethylfurfural, in deep eutectic solvents, in the presence of acidic task-specific ionic liquids as catalysts. We employed aliphatic and aromatic ionic liquids as catalysts, and choline chloride-based deep eutectic solvents bearing glycols or carboxylic acids, as solvents. The reactions were performed in a biphasic system, with acetone as a benign extracting solvent, enabling continuous extraction of 5-HMF. We aimed to find the best experimental conditions for this transformation, in terms of catalyst loading, solvent, reaction time and temperature to achieve an economical and energy efficient process. We also analyzed the results in terms of solvent viscosity and structural organization as well as catalysts acidity, to elucidate which structural features mostly favour the reaction. Under optimized conditions, we obtained a yield in 5-HMF of 71 %, at 80 °C in 3 h. Our system can be scaled up and recycled three times with no loss in yield. Finally, comparison with the literature shows that our system achieves a higher yield under milder conditions than most protocols so far reported for the same transformation.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402522"},"PeriodicalIF":7.5,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031510","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemSusChemPub Date : 2025-01-24DOI: 10.1002/cssc.202402178
Wen Ou, Donghua Liu, Xin Ye, Ningyi Cui, Yecheng Zhou
{"title":"Revealing the Surface Reconstruction on the High OER Catalytic Activity of Ni3S2.","authors":"Wen Ou, Donghua Liu, Xin Ye, Ningyi Cui, Yecheng Zhou","doi":"10.1002/cssc.202402178","DOIUrl":"https://doi.org/10.1002/cssc.202402178","url":null,"abstract":"<p><p>Sluggish oxygen evolution reaction (OER) is a crucial part of water splitting and solar fuel generation, which limits their utilization. Ni3S2 is a promising OER catalyst, in which surface reconstruction is an important step to improve performance. In this study, DFT calculations were employed to investigate the effect of surface reconstruction on (001), (110), and (101) surfaces of Ni3S2 in alkaline OER. According to the Pourbaix diagram and surface free energy landscape, Ni3S2 is prone to transform into Ni oxides and (oxy) hydroxides under alkaline OER conditions. This process induces exposed S atoms to leach and O from the electrolyte to incorporate S sites, thereby lowering the Bader charge of *O and increasing [[EQUATION]], and then decrease [[EQUATION]], the free energy penalty of the potential determining step. In general, the surface reconstruction enhances the OER activity through S leaching and adjusting the coordination environment. We believe this work not only provides insights into the clarification of surface reconstruction, but also provides a valuable guideline for the further discovery of efficient TM-based sulfides.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402178"},"PeriodicalIF":7.5,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031581","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemSusChemPub Date : 2025-01-24DOI: 10.1002/cssc.202402513
YuKe Su, Suqin Liu, Weiwei Zhu, Kui Huang, Guangyuan Mu, Peng Jiang, Jianhui Liu, Guang Yang, Zhen He, Jue Wang
{"title":"Nature of Solvent/Nonsolvent Strategy in Achieving Superior Polybenzimidazole Membrane for Vanadium Redox Flow Battery.","authors":"YuKe Su, Suqin Liu, Weiwei Zhu, Kui Huang, Guangyuan Mu, Peng Jiang, Jianhui Liu, Guang Yang, Zhen He, Jue Wang","doi":"10.1002/cssc.202402513","DOIUrl":"https://doi.org/10.1002/cssc.202402513","url":null,"abstract":"<p><p>The tightly connected structure of polybenzimidazole (PBI) membrane can be relaxed by solvent/nonsolvent solution to achieve a high proton conductivity for vanadium redox flow battery (VRFB). However, the nature behind the solvent/nonsolvent strategy is not unraveled. This work proposes a guideline to analyze the effect of PBI membrane relaxing formulas based on the interactions between different components in membranes. The supreme-efficient PBI membrane derived by the DMSO/formamide formula according to the guideline displays a marvelous performance for VRFB, with the proton conductivity boosted by 4300% (from 1.93 to 83.33 mS cm-1), and VRFB assembled with this membrane achieves an outstanding energy efficiency of 82.5% under 200 mA cm-2. Moreover, this work profoundly unravels the structure, property and performance relationship of PBI membrane, which is of great value for the development of membranes.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402513"},"PeriodicalIF":7.5,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031513","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Size-Dependency of Electrochemically Grown Copper Nanoclusters Derived from Single Copper Atoms for the CO Reduction Reaction.","authors":"Keitaro Ohashi, Kosei Nishimura, Kaito Nagita, Takuya Hashimoto, Shoko Nakahata, Takashi Harada, Toshiaki Ina, Shuji Nakanishi, Kazuhide Kamiya","doi":"10.1002/cssc.202402576","DOIUrl":"https://doi.org/10.1002/cssc.202402576","url":null,"abstract":"<p><p>Electrochemically grown copper nanoclusters (CuNCs: < 3 nm) from single-atom catalysts have recently attracted intensive attention as electrocatalysts for CO2 and CO reduction reaction (CO2RR/CORR) because they exhibit distinct product selectivity compared with conventional Cu nanoparticles (typically larger than 10 nm). Herein, we conducted a detailed investigation into the size dependence of CuNCs on selectivity for multicarbon (C2+) production in CORR. These nanoclusters were electrochemically grown from single Cu atoms dispersed on covalent triazine frameworks (Cu-CTFs). Operando X-ray absorption fine structure analysis revealed that Cu-CTFs containing 1.21 wt% and 0.41 wt% Cu (Cu(h)-CTFs and Cu(l)-CTFs, respectively) formed CuNCs of 2.0 and 1.1 nm, respectively, at -1.0 V vs. RHE. The selectivity for CORR products was particularly dependent on the size of CuNCs, with the Faraday efficiencies of C2+ products being 52.3% and 32.7% at -1.0 V vs. RHE with Cu(h)-CTFs and Cu(l)-CTFs, respectively. Spherical CuNCs modeling revealed that larger cluster sizes led to a greater proportion of a surface coordination number (SCN) of 8 or 9. Density functional calculations revealed that the CO dimerization reaction was more likely to proceed at SCNs of 8 or 9 compared to SCN of 7 because of the stability of the *OCCO intermediate.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402576"},"PeriodicalIF":7.5,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031584","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemSusChemPub Date : 2025-01-24DOI: 10.1002/cssc.202402563
Jie Ma, Shuzhen Liang, Xue Yang, Yabo Wang, Bingzheng Wang, Wei Gao, Kang Ye, Mairemu Maihaiti, Javed Iqbal, Abdukader Abdukayum, Fanghui Pan
{"title":"Design of Carbon Materials with Selective Ion Separation in Capacitive Deionisation and Their Applications.","authors":"Jie Ma, Shuzhen Liang, Xue Yang, Yabo Wang, Bingzheng Wang, Wei Gao, Kang Ye, Mairemu Maihaiti, Javed Iqbal, Abdukader Abdukayum, Fanghui Pan","doi":"10.1002/cssc.202402563","DOIUrl":"https://doi.org/10.1002/cssc.202402563","url":null,"abstract":"<p><p>Capacitive deionization (CDI) is a novel, cost-effective and environmentally friendly desalination technology that has garnered significant attention in recent years. Carbon materials, owing to their excellent properties, have become the preferred electrode materials for CDI. Given the significant differences between different ions, ion-selective performance has emerged as a critical aspect of CDI applications. However, comprehensive reviews on the selective ion separation capabilities of carbon materials for CDI remain scarce. This review examines the progress in developing carbon materials for ion-selective separation in CDI, focusing on regulatory mechanisms and representative materials. It also discusses the applications of selective CDI carbon materials in areas such as heavy metal removal, nutrient recovery, seawater desalination resourcing, and water softening. Furthermore, the challenges and future prospects for advancing carbon materials in CDI are explored. This review aims to provide theoretical insights and practical guidance for utilising carbon materials in wastewater treatment and resource recovery.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402563"},"PeriodicalIF":7.5,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031508","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemSusChemPub Date : 2025-01-23DOI: 10.1002/cssc.202402485
Yuqi Ren, Shengnan Lan, Yuan-Hao Zhu, Ruoxuan Peng, Hongbin He, Yitao Si, Kai Huang, Naixu Li
{"title":"Concentrated Solar-Driven Catalytic CO2 Reduction: From Fundamental Research to Practical Applications.","authors":"Yuqi Ren, Shengnan Lan, Yuan-Hao Zhu, Ruoxuan Peng, Hongbin He, Yitao Si, Kai Huang, Naixu Li","doi":"10.1002/cssc.202402485","DOIUrl":"https://doi.org/10.1002/cssc.202402485","url":null,"abstract":"<p><p>Concentrated solar-driven CO2 reduction is a breakthrough approach to combat climate crisis. Harnessing the in-situ coupling of high photon flux density and high thermal energy flow initiates multiple energy conversion pathways, such as photothermal, photoelectric, and thermoelectric processes, thereby enhancing the efficient activation of CO2. This review systematically presents the fundamental principles of concentrated solar systems, the design and classification of solar-concentrating devices, and industrial application case studies. Meanwhile, key technological advances-from theoretical foundations to practical applications-are also discussed. At the microscopic level, a comprehensive analysis of multiscale reaction kinetics within the domain of photothermal synergistic catalysis has been conducted. This analysis elucidates the significance of catalyst design, further detailing the intricate regulatory mechanisms governing reaction pathways and active sites through nanostructured catalysts, single-atom catalysts, and metal-support interactions. However, the transition from laboratory research to industrial-scale application still faces challenges, including the complexity of system integration, energy density optimization, and economic feasibility. This review provides a theoretical framework and practical guidance through a complete investigation of current technological bottlenecks and future development directions, with the aim of driving key advances in concentrated solar-driven CO2 reduction catalysis.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402485"},"PeriodicalIF":7.5,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143021339","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"2D/3D heterojunction engineering for hole transport layer-free carbon-based perovskite solar cells.","authors":"Lingcong Li, Yinlong Lai, Huashang Rao, Weizi Cai, Xinhua Zhong, Huishi Guo, Zhenxiao Pan","doi":"10.1002/cssc.202402549","DOIUrl":"https://doi.org/10.1002/cssc.202402549","url":null,"abstract":"<p><p>Hole transport layer (HTL)-free carbon-based perovskite solar cells (C-PSCs) own outstanding potential for commercial applications due to their attractive advantages of low cost and superior stability. However, the abundant defects and mismatched energy levels at the interface of the perovskite/carbon electrode severely limit the device efficiency and stability. Constructing a 2D layer on the surface of 3D perovskite films to form 2D/3D heterojunctions has been demonstrated to be an effective method of passivating surface defects and optimizing the energy level alignment in almost all kinds of PSCs. Due to the unique structure of HTL-free C-PSCs, 2D/3D heterojunctions play especially important roles. This review article summarizes the reports of 2D/3D perovskite heterojunctions in HTL-free C-PSCs. It describes the contributions of 2D/3D heterojunctions in terms of their roles in defect passivation, energy level optimization, and stability improvement. Finally, challenges and prospects of 2D/3D heterojunction for further development of HTL-free C-PSCs are highlighted.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402549"},"PeriodicalIF":7.5,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031506","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ChemSusChemPub Date : 2025-01-23DOI: 10.1002/cssc.202402237
Lorena Alcaraz, Olga Rodríguez-Largo, Gorka Barquero-Carmona, Alba Berja, Adrián Quesada, Félix A López
{"title":"Recovery of rare earths from end-of-life NdFeB permanent magnets from wind turbines.","authors":"Lorena Alcaraz, Olga Rodríguez-Largo, Gorka Barquero-Carmona, Alba Berja, Adrián Quesada, Félix A López","doi":"10.1002/cssc.202402237","DOIUrl":"https://doi.org/10.1002/cssc.202402237","url":null,"abstract":"<p><p>This work aims to recover rare earths from wind turbines NdFeB magnets through pyrometallurgical and hydrometallurgical techniques. First, a NdFeB hydride powder is obtained by decrepitation with hydrogen. Subsequently, this powder was subjected to a chlorination roasting process and successive leaching with water to bring the metals into solution. This was followed by a liquid-liquid extraction to remove the iron and purify the rare earth solution. For this purpose, Aliquat 336 diluted in Solvesso was selected as the iron selective extraction agent. As a single extraction was not enough for complete iron removal, a second Fe extraction step was carried out. This second extraction step was performed using the restored organic phase. This restoration was achieved by treating the organic phase with Na2SO3 and then washing it with a 3M HCl solution. In this way, the process was achieved more sustainably. Finally, the rare earths contained in the final solution were precipitated using oxalic acid to obtain mixed rare earth oxalates.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402237"},"PeriodicalIF":7.5,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031578","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}