ChemSusChemPub Date : 2025-03-17DOI: 10.1002/cssc.202402769
Yao Dai, Kaihang Yue, Yingjie Wan, Peng Zhao, Yongwen Tan, Fuqiang Huang, Ya Yan
{"title":"Efficient and Stable Acidic Oxygen Evolution Based on W<sub>18</sub>O<sub>49</sub> Nanowires Supported IrO<sub>X</sub>.","authors":"Yao Dai, Kaihang Yue, Yingjie Wan, Peng Zhao, Yongwen Tan, Fuqiang Huang, Ya Yan","doi":"10.1002/cssc.202402769","DOIUrl":"10.1002/cssc.202402769","url":null,"abstract":"<p><p>Proton exchange membrane water electrolyzer (PEMWE) is considered to be a promising green hydrogen production technology but place high demand on the anodic oxygen-evolving electrocatalysts to withstand the strong oxidizing and acidic reaction condition. Here we report a robust W<sub>18</sub>O<sub>49</sub> nanowire supported IrO<sub>X</sub> (IrO<sub>X</sub>-W<sub>18</sub>O<sub>49</sub>) catalyst for acidic oxygen evolution reaction (OER) prepared by chemical vapor deposition followed with polyol reduction. The catalyst exhibits excellent electrocatalytic OER performance with an overpotential of 223 mV for a current density of 10 mA cm<sup>-2</sup> and a small Tafel slope of 66.4 mV dec<sup>-1</sup> in acidic media, superior to most electrocatalysts. More impressively, the assembled three-electrode cell with IrO<sub>X</sub>-W<sub>18</sub>O<sub>49</sub> as the working electrode exhibits excellent electrocatalytic OER performance and can operate stably at 10 mA cm<sup>-2</sup> for 140 h. In-situ spectroscopy characterizations reveal that the IrO<sub>X</sub>-W<sub>18</sub>O<sub>49</sub> works in a route of lattice oxygen mechanism during OER. The favorable interaction between W<sub>18</sub>O<sub>49</sub> nanowires and the IrO<sub>X</sub> active species together with the strong Ir-O interaction stabilizes the high-valence Ir and prolongs the service life of the catalyst for OER.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402769"},"PeriodicalIF":7.5,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143646701","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 : 2025-03-17DOI: 10.1002/cssc.202402218
Francesco Tavola, Gian Pietro De Gaudenzi, Giulio Bidinotto, Francesco Casamichiela, Andrea Pola, Sandra Tedeschi, Benedetto Bozzini
{"title":"Efficient and Sustainable Electrochemical Demolition of Hard-Metal Scrap with Co-Rich Binder.","authors":"Francesco Tavola, Gian Pietro De Gaudenzi, Giulio Bidinotto, Francesco Casamichiela, Andrea Pola, Sandra Tedeschi, Benedetto Bozzini","doi":"10.1002/cssc.202402218","DOIUrl":"https://doi.org/10.1002/cssc.202402218","url":null,"abstract":"<p><p>Cobalt and tungsten hold strategic importance in various industries, and fostering their circular economy could lead to cost reduction and a more sustainable use of natural resources. Eco- friendly electrochemical recovering processes are promising alternatives to the state-of-the-art pyrometallurgical approaches, but their productivity is too low for industrial standards. Low demolition rates are caused by hardmetal pseudopassivation phenomena. In previous work, we demonstrated that a pulsed-potential approach, employing a neutral aqueous solution and alternating pseudopassivating film formation with its mechanical removal by oxygen evolution reaction, thus refreshing an active HM surface, is effective in avoiding the corrosion-self-termination for corrosion-resistant grades. This study extends this approach to the most widespread grades, featuring Co-rich binders. This new application required fine-tuning of the operating conditions to adapt them to the target grades. Electrochemical characterization of the psudopassive film growth in this study is centered on cyclic voltammetry and potentiostatic polarization. Corroded hardmetal and detached pseudopassive films were subjected to morphological and compositional analyses with scanning electron microscopy and x-ray fluorescence mapping. We thus demonstrated that optimized pulsed anodic potentiostatic polarization enables efficient demolition of hard metal coupons, combined with separation of Co and W, at high rate and with low energy consumption.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402218"},"PeriodicalIF":7.5,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143646705","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 : 2025-03-17DOI: 10.1002/cssc.202500303
Pauline Blyweert, Ana R Querido, Olivia S G P Soares, Vincent Nicolas, Vanessa Fierro, Manuel F R Pereira, Alain Celzard
{"title":"Exploring CO<sub>2</sub> Methanation Using 3D-Printed Carbon Architectures.","authors":"Pauline Blyweert, Ana R Querido, Olivia S G P Soares, Vincent Nicolas, Vanessa Fierro, Manuel F R Pereira, Alain Celzard","doi":"10.1002/cssc.202500303","DOIUrl":"https://doi.org/10.1002/cssc.202500303","url":null,"abstract":"<p><p>To demonstrate for the first time the potential of stereolithography-printed, architected, bio-based carbon-supported Ni catalysts for CO<sub>2</sub> methanation, three honeycomb carbon structures with different textural properties were prepared, impregnated with 15 wt.% of nickel metal particles, and studied to correlate their catalytic performances with their textural properties and surface chemistry. Compared with the non-activated monolith and the steam-activated monolith, the CO<sub>2</sub>-activated monolith achieved a higher CO<sub>2</sub> conversion of 62 % with a CH<sub>4</sub> selectivity of 73 % at 460 °C. Our comparative study demonstrated that the CO<sub>2</sub>-activated carbon support, although having fewer basic sites on the surface, exhibits greater dispersion of the Ni phase, enabling an increase in H<sub>2</sub> chemisorption. These results are of interest for further studies related to the optimization of catalytic performance through the design of the architectural and textural properties of such macrostructures.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500303"},"PeriodicalIF":7.5,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143646710","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 : 2025-03-16DOI: 10.1002/cssc.202500032
Sayanti Chatterjee, Arya Singh, Yashdeep Maurya, Akhilesh Sharma, V S Swetha, Mehar Ul Nisa, Vishal Kumar, Puneet Gupta, Kartikay Tyagi
{"title":"An Iron-Catalyzed Sustainable Functional Group Transfer Strategy for In-Water Transformation of Organic Sulfides to Sulfoxides by a Hydroxylamine Derived Oxidant.","authors":"Sayanti Chatterjee, Arya Singh, Yashdeep Maurya, Akhilesh Sharma, V S Swetha, Mehar Ul Nisa, Vishal Kumar, Puneet Gupta, Kartikay Tyagi","doi":"10.1002/cssc.202500032","DOIUrl":"https://doi.org/10.1002/cssc.202500032","url":null,"abstract":"<p><p>An unprecedented strategy for unlocking a new and efficient functional group transfer protocol has been demonstrated to synthesize a variety of complex organic sulfoxides chemoselectively, starting from organic sulfides. The strategy of this new functional group transfer protocol is based on harnessing the potential of metalloradical-assisted intermolecular functional group transposition or 'InterGroupXfer' to replace highly sensitive and reactive high valent metal intermediates, [M=X] (X = O, NH).This sustainable functional group transfer strategy employs earth abundant iron catalyst and bench-stable and convenient-to-handle hydroxyl amine derived surrogate, operates under mild conditions in water or even under solvent free condition, exhibits broad functional group tolerance, as well as versatility of reaction scale and proceeds without the use of any precious metal catalyst or additional oxidant. A comprehensive electronic and mechanistic investigation, supported by DFT calculations, has been conducted to elucidate the reaction mechanism. The utility of the developed methodology as well as studies of biological activity foster future pathways for exploring uncharted chemical space. The reported work with exceptional synthetic flexibility and operational simplicity aligns well with the prospect of green and sustainable chemistry and is expected to unlock new avenue in the emerging research area of catalytic functional group transfer reactivity.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500032"},"PeriodicalIF":7.5,"publicationDate":"2025-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143639387","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":"A Scalable Strategy of \"Ball-Milling-Assisted Laser Scanning Method\" to Achieve Cr<sub>2</sub>Ni<sub>3</sub> Catalyst: An Unprecedented Robust Anode for Oxygen Evolution Reaction.","authors":"Yingli Ren, Mingyu Su, Shengli Zhu, Zhenduo Cui, Zhaoyang Li, Shuilin Wu, Wence Xu, Zhonghui Gao, Yanqin Liang, Lili Ma, Hui Jiang","doi":"10.1002/cssc.202500140","DOIUrl":"10.1002/cssc.202500140","url":null,"abstract":"<p><p>Industrial water-alkali splitting is facing high energy consumption due to the high overpotential of commercial Ni mesh anode in oxygen evolution reaction (OER) processing. Herein, a simple ball-milling-assisted laser scanning strategy was employed to introduce the hardest Lewis acid chromium (Cr) into the Ni matrix to form Cr2Ni3 catalysts supported by Ni mesh, endowing such NiCr/Ni mesh anode a robust OER performance at a low-cost. It is shown that facilitating the self-adsorption of oxygen species and promoting the leaching of soluble Cr cations aids in reconstructing Ni cations into active (oxy)hydroxide species. This study explores the innovative development of Cr-doped NiCr/Ni mesh catalysts to create porous NiCr/Ni alloys with Cr2Ni3 as the active phase. The optimal Ni<sub>0.5</sub>Cr<sub>0.5</sub>-NM electrode demonstrates ultra-low overpotentials of 293 mV and 321 mV at 50 and 100 mA cm<sup>-2</sup>, respectively, while maintaining excellent stability for over 100 hours at 100 mA cm<sup>-2</sup>. This work provides insight into the batch fabrication of customized OER anodes for sustainable hydrogen production.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500140"},"PeriodicalIF":7.5,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143633270","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":"Reactor for Photocatalytic Hydrogen Production from Water.","authors":"Xin-Yu Meng, Tingwei Wang, Jin-Jin Li, Chih-Chun Ching, Yin-Ning Zhou, Yun-Xiang Pan","doi":"10.1002/cssc.202500317","DOIUrl":"10.1002/cssc.202500317","url":null,"abstract":"<p><p>Solar-energy-driven photocatalytic water (H<sub>2</sub>O) splitting converts solar energy into a high-valuable chemical, i. e. hydrogen (H<sub>2</sub>), and is thereby a promising technique for achieving a sustainable society. However, photocatalytic H<sub>2</sub>O splitting have not been applied at a scalable industrial level yet. In addition to photocatalyst, reactor is also a crucial factor affecting efficiency of photocatalytic H<sub>2</sub>O splitting. There are a large number of works focusing on photocatalytic H<sub>2</sub>O splitting, including both reviews and research works. However, the reported works on photocatalytic H<sub>2</sub>O splitting paid little attentions on reactor. Herein, we discuss recent progresses on reactor for photocatalytic H<sub>2</sub>O splitting, and highlight challenges for further studies. This is helpful for further improving efficiency of photocatalytic H<sub>2</sub>O splitting.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500317"},"PeriodicalIF":7.5,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143629989","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 : 2025-03-14DOI: 10.1002/cssc.202500361
Peizhi Dong, Huiqing Fan, Lin Lei, Yongbo Fan, Shimiao Tang, Ruizhe Zhang, Zhiyong Liao, Zhuo Zhang, Ning Yang, Zexue Lin, Weijia Wang
{"title":"Vapor deposition assisted in-situ construction of graphitic carbon nitride homojunction capable of enhanced visible-light-driven hydrogen generation.","authors":"Peizhi Dong, Huiqing Fan, Lin Lei, Yongbo Fan, Shimiao Tang, Ruizhe Zhang, Zhiyong Liao, Zhuo Zhang, Ning Yang, Zexue Lin, Weijia Wang","doi":"10.1002/cssc.202500361","DOIUrl":"https://doi.org/10.1002/cssc.202500361","url":null,"abstract":"<p><p>Graphitic carbon nitride (g-C3N4) has garnered considerable attention in the field of photocatalysis due to its suitable bandgap (~2.7 eV), abundant elemental composition, high chemical stability, and environmentally friendly synthesis process. In this study, a novel g-C3N4 homojunction material with controllable morphology was successfully fabricated via a simple and efficient vapor deposition method. Under visible light irradiation, this material demonstrated exceptional photocatalytic hydrogen evolution performance, achieving a hydrogen production rate of 334 μmol g-1 h-1, approximately 24 times higher than that of conventional bulk g-C3N4. This remarkable enhancement in performance can be attributed to the synergistic effects of several factors, including a significant increase in specific surface area, expanded visible-light absorption range, efficient separation and migration of photogenerated charge carriers, and the coupling effect of optimized band structure and crystal morphology. This study not only provides new insights for further enhancing the photocatalytic performance of CN-based materials but also lays a solid foundation for their practical applications in sustainable energy and environmental remediation.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500361"},"PeriodicalIF":7.5,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143622909","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":"Alloying Engineering of Defective Molybdenum Sulfide Basal Planes for Enhanced Borrowing Hydrogen Activity in the Thioetherification of Alcohols.","authors":"Miriam Rodenes, Darija Oštrić, Santiago Martín, Patricia Concepción, Avelino Corma, Iván Sorribes","doi":"10.1002/cssc.202500343","DOIUrl":"10.1002/cssc.202500343","url":null,"abstract":"<p><p>The borrowing hydrogen thioetherification of alcohols over heterogeneous catalysts has emerged as an attractive and practical synthetic strategy to prepare thioethers from the perspective of green and sustainable chemistry. Developing efficient catalysts is the key to improve this carbon-sulfur (C-S) bond formation process. Herein, a novel catalyst, namely {Mo<sub>2.89</sub>W<sub>0.11</sub>S<sub>4</sub>}<sub>n</sub>, has been prepared by alloying engineering of its basal planes through an innovative synthetic methodology that makes use of isostructural building entities based on molybdenum and tungsten sulfide molecular complexes with M<sub>3</sub>S<sub>4</sub> (M=Mo, W) cluster cores. Besides excellent activity and reusability, {Mo<sub>2.89</sub>W<sub>0.11</sub>S<sub>4</sub>}<sub>n</sub> is of broad scope, enabling the conversion of structurally diverse thiols and primary as well as secondary alcohols into thioethers. A set of characterizations, in combination with catalytic results, reveal that the catalytic activity of {Mo<sub>2.89</sub>W<sub>0.11</sub>S<sub>4</sub>}<sub>n</sub> for this relevant transformation arises from the presence of multiple-type active centers in the defective basal planes of this alloyed catalyst. More specifically, coordinatively unsaturated sulfurs and metal atoms with Lewis basic and Lewis acid properties, respectively, are proposed to be the active sites involved in the borrowing hydrogen mechanism.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500343"},"PeriodicalIF":7.5,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143622902","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 : 2025-03-13DOI: 10.1002/cssc.202402566
Parker Ballard-Kyle, Isabel Hsieh, Huiyuan Zhu
{"title":"Electrocatalytic C-N Coupling: Advances in Urea Synthesis and Opportunities for Alternative Products.","authors":"Parker Ballard-Kyle, Isabel Hsieh, Huiyuan Zhu","doi":"10.1002/cssc.202402566","DOIUrl":"https://doi.org/10.1002/cssc.202402566","url":null,"abstract":"<p><p>Urea is an essential fertilizer produced through the industrial synthesis of ammonia (NH3) via the Haber-Bosch process, which contributes approximately 1.2% of global annual CO2 emissions. Electrocatalytic urea synthesis under ambient conditions via C-N coupling from CO2 and nitrogen species such as nitrate (NO3-), nitrite (NO2), nitric oxide (NO), and nitrogen gas (N2) -has gained interest as a more sustainable route. However, challenges remain due to the unclear reaction pathways for urea formation, competing reactions, and the complexity of the resulting product matrix. This review highlights recent advances in catalyst design, urea quantification, and intermediate identification in the C-N coupling reaction for electrocatalytic urea synthesis. Furthermore, this review explores future prospects for industrial C-N coupling, considering potential nitrogen and carbon sources and examining alternative C-N coupling products, such as amides and amines.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402566"},"PeriodicalIF":7.5,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143622906","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":"Non-copper-based Catalysts for CO<sub>2</sub> Electroreduction to Multi-carbon Compounds.","authors":"Zhouhui Chen, Wanfu Zhong, Chunyuan Shi, Weihang Tang, Qinghong Zhang, Ye Wang, Shunji Xie","doi":"10.1002/cssc.202402755","DOIUrl":"10.1002/cssc.202402755","url":null,"abstract":"<p><p>Renewable energy has made significant strides, with the cost of clean electricity plummeting, making the use of renewable electricity for electrocatalytic CO<sub>2</sub> reduction to synthesize high-value chemicals and fuels more economically attractive. Notably, certain non-copper-based electrocatalysts have shown remarkable selectivity for C<sub>2+</sub> products at low overpotentials, even enabling the production of multi-carbon molecules that are undetectable on copper-based electrodes. This breakthrough opens up new avenues for research into non-copper catalysts. This article offers a thorough review of the latest research progress in employing non-copper-based catalysts for CO<sub>2</sub> conversion, focusing on the generation of C<sub>2+</sub> products in aqueous media. It explores the complex mechanisms of carbon-carbon coupling and provides a critical assessment of future directions for improving catalyst design, modulating interface microenvironments, and optimizing reaction systems for non-copper-based catalysts in CO<sub>2</sub> reduction reactions (CO<sub>2</sub>RR).</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402755"},"PeriodicalIF":7.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143603062","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}