ChemSusChemPub Date : 2024-10-23DOI: 10.1002/cssc.202401100
Huixuan Cao, Ge Chen, Yong Yan, Dong Wang
{"title":"Advances in Two-Electron Water Oxidation Reaction for Hydrogen Peroxide Production: Catalyst Design and Interface Engineering.","authors":"Huixuan Cao, Ge Chen, Yong Yan, Dong Wang","doi":"10.1002/cssc.202401100","DOIUrl":"https://doi.org/10.1002/cssc.202401100","url":null,"abstract":"<p><p>Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) is a versatile and zero-emission material that is widely used in the industrial, domestic, and healthcare sectors. It is clear that it plays a critical role in advancing environmental sustainability, acting as a green energy source, and protecting human health. Conventional production techniques focused on anthraquinone oxidation, however, electrocatalytic synthesis has arisen as a means of utilizing renewable energy sources in conjunction with available resources like oxygen and water. These strides represent a substantial change toward more environmentally and energy-friendly H<sub>2</sub>O<sub>2</sub> manufacturing techniques that are in line with current environmental and energy goals. This work reviews recent advances in two-electron water oxidation reaction (2e-WOR) electrocatalysts, including design principles and reaction mechanisms, examines catalyst design alternatives and experimental characterization techniques, proposes standardized assessment criteria, investigates the impact of the interfacial milieu on the reaction, and discusses the value of in situ characterization and molecular dynamics simulations as a supplement to traditional experimental techniques and theoretical simulations, as shown in Figure 1. The review also emphasizes the importance of device design, interface, and surface engineering in improving the production of H<sub>2</sub>O<sub>2</sub>. Through adjustments to the chemical microenvironment, catalysts can demonstrate improved performance, opening the door for commercial applications that are scalable through tandem cell development.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401100"},"PeriodicalIF":7.5,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491590","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 : 2024-10-23DOI: 10.1002/cssc.202401865
Qiuyue Li, Jingjing Liu, Ze Wu, Aomeng Deng, Jiani Liu, Tian Chen, Jianlong Wei, Yiqiong Zhang, Hanwen Liu
{"title":"Recent Advances in Electrocatalytic C-N Coupling for Urea Synthesis.","authors":"Qiuyue Li, Jingjing Liu, Ze Wu, Aomeng Deng, Jiani Liu, Tian Chen, Jianlong Wei, Yiqiong Zhang, Hanwen Liu","doi":"10.1002/cssc.202401865","DOIUrl":"10.1002/cssc.202401865","url":null,"abstract":"<p><p>Urea, one of the most widely used nitrogen-containing fertilizers globally, is essential for sustainable agriculture. Improving its production is crucial for meeting the increasing demand for fertilizers. Electrocatalytic co-reduction of CO₂ and nitrogenous compounds (NO₂<sup>-</sup>/NO₃<sup>-</sup>) has emerged as a promising strategy for green and energy-efficient urea synthesis. However, challenges such as slow reaction kinetics and complex multi-step electron transfers have hindered the development of efficient urea synthesis methods. This review explores recent advances in the electrocatalytic C-N coupling process, focusing on bimetallic catalysts, metal oxide/hydroxide catalysts, and carbon-based catalysts. The review also discusses the future prospects of designing effective catalysts for electrocatalytic C-N coupling to improve urea synthesis.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401865"},"PeriodicalIF":7.5,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491607","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 : 2024-10-22DOI: 10.1002/cssc.202401849
Denis A Kolykhalov, Anastasia N Golysheva, Kirill S Erokhin, Bogdan Ya Karlinskii, Valentine P Ananikov
{"title":"The Stability Challenge of Furanic Platform Chemicals in Acidic and Basic Conditions.","authors":"Denis A Kolykhalov, Anastasia N Golysheva, Kirill S Erokhin, Bogdan Ya Karlinskii, Valentine P Ananikov","doi":"10.1002/cssc.202401849","DOIUrl":"10.1002/cssc.202401849","url":null,"abstract":"<p><p>The transition toward renewable resources is pivotal for the sustainability of the chemical industry, making the exploration of biobased furanic platform chemicals derived from plant biomass of paramount importance. These compounds, promising alternatives to petroleum-derived aromatics, face challenges in terms of stability under synthetic conditions, limiting their practical application in the fuel, chemical, and pharmaceutical sectors. Our study presents a comprehensive evaluation of the stability of furan derivatives in various solvents and under different conditions, addressing the significant challenge of their instability. Through systematic experiments involving GC-MS, NMR, FT-IR and SEM analyses, we identified key degradation pathways and conditions that either promote stability or lead to undesirable degradation products. These findings demonstrate the strong stabilizing effect of polar aprotic solvents, especially DMF, and reveal the dependence of furan stability on solvent and additive type. This research opens new avenues in the utilization of renewable furans by providing critical insights into their behavior under synthetic conditions, significantly impacting the development of sustainable materials and processes. The broad appeal of this study lies in its potential to guide the selection of conditions for the efficient and sustainable synthesis of furan-based chemicals, marking a significant advance in green chemistry and materials science.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401849"},"PeriodicalIF":7.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491610","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 : 2024-10-22DOI: 10.1002/cssc.202401170
Joost M van Gaalen, J Chris Slootweg
{"title":"From Critical Raw Materials to Circular Raw Materials.","authors":"Joost M van Gaalen, J Chris Slootweg","doi":"10.1002/cssc.202401170","DOIUrl":"https://doi.org/10.1002/cssc.202401170","url":null,"abstract":"<p><p>This perspective addresses the key challenge of advancing the use of Critical Raw Materials (CRMs) and proposes a transition towards circular raw material management. In the context of our current economy, the unsustainable consumption, environmental degradation, geopolitical risks, and economic vulnerabilities associated with CRMs highlight the limitations in ensuring long-term CRM availability, emphasizing the environmental, social, and economic implications. In response, this perspective underlines a multifaceted technological approach to mitigate CRM criticality, focusing on reducing CRM use, substituting CRMs with less critical materials, and enhancing recovery and recycling processes, with Design for Circularity as the most impactful solution. The latter advocates for a paradigm shift in product design and material utilization, emphasizing principles like modular design, product life extension, and the transition from product ownership to service models. Such a holistic approach is not only crucial for sustainable CRM management, but is also key to fostering a resilient and low-carbon economy.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401170"},"PeriodicalIF":7.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491603","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 : 2024-10-22DOI: 10.1002/cssc.202401678
Ruiyong Chen
{"title":"New Redox Chemistries of Halogens in Aqueous Batteries.","authors":"Ruiyong Chen","doi":"10.1002/cssc.202401678","DOIUrl":"10.1002/cssc.202401678","url":null,"abstract":"<p><p>Halogen-based redox-active materials represent an important class of materials in aqueous electrochemistry. The existence of versatile halogen species and their rich bonding coordination create great flexibility in designing new redox couples. Novel redox reaction mechanisms and electrochemical reversibility can be unlocked in specifically configurated electrolyte environments and electrodes. In this review, the halogen-based redox couples and their appealing redox chemistries in aqueous batteries, including redox flow batteries and traditional static batteries that have been studied in recent years, are discussed. New aqueous electrochemistry provides hope to outperform the state-of-the-art materials and systems that are facing resources and performance limitation, and to enrich the existing battery chemistries.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401678"},"PeriodicalIF":7.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142454154","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 : 2024-10-22DOI: 10.1002/cssc.202401578
Ziyao Liu, Faiza Siddique, Yan Wei, Md Ariful Haque, Li Na, Xiaofeng Yang, Carol Sze Ki Lin
{"title":"Efficient Production of Bacterial Cellulose Using Komagataeibacter sucrofermentans on Sustainable Feedstocks.","authors":"Ziyao Liu, Faiza Siddique, Yan Wei, Md Ariful Haque, Li Na, Xiaofeng Yang, Carol Sze Ki Lin","doi":"10.1002/cssc.202401578","DOIUrl":"10.1002/cssc.202401578","url":null,"abstract":"<p><p>The production of bacterial cellulose (BC) has indeed garnered global attention due to its versatile properties and applications. Despite potential benefits, the challenges like low productivity, high fermentation costs, and expensive culture media hinder its industrialization. Utilizing low-cost substrates, especially waste streams, can help address the challenges. In this study, waste feedstocks such as restaurant leftovers, oranges, and grapefruit from canteens and supermarkets were valorized for BC production by Komagataeibacter sucrofermentans. Orange juice is a fascinating substrate with a highest concentration of 20.6 g/L and productivity of 2.05 g/L/d. Using HS medium with supplementary ions, organic acids, ethanol, and various carbon sources is a strategic approach for enhancing BC production. The study reveals that the addition of organic acids or ethanol moderately increased BC production, while ions inhibit BC synthesis, highlighting the complex interplay between various cultivation medium components. Additionally, fermentation with K. sucrofermentans using single and mixed carbon sources was conducted to elucidate the potential metabolic mechanism of BC production. Through alkaline treatment and drying in a 30 °C incubator, we produced the highest quality BC with 92.09 % crystallinity. Overall, the study enhances BC production knowledge and provides green and sustainable strategies for fermentative BC production.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401578"},"PeriodicalIF":7.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491595","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 : 2024-10-22DOI: 10.1002/cssc.202401701
Rajib Maity, Sudipta Paul, Anupam Sen, Sukla Garain, Biplab Maji
{"title":"Electricity-Driven Strain-Release Cascade Cyclization of Bicyclo[1.1.0]butane (BCB): Stereoselective Synthesis of Functionalized Spirocyclobutyl Oxindoles.","authors":"Rajib Maity, Sudipta Paul, Anupam Sen, Sukla Garain, Biplab Maji","doi":"10.1002/cssc.202401701","DOIUrl":"10.1002/cssc.202401701","url":null,"abstract":"<p><p>Spirocyclobutyl oxindoles, characterized by their unique three-dimensional structures, are valuable building blocks for many pharmacophores and drug units. However, stereoselective synthetic strategies for these scaffolds remain underdeveloped, with most existing methods relying on transition metal catalysts and stoichiometric redox reagents. In this work, we introduce an electrochemical strain-release driven cascade spirocyclization of bicyclo[1.1.0]butane (BCB) derivatives for the stereoselective synthesis of functionalized spirocyclobutyl oxindoles. Tetrabutylammonium bromide serves a dual purpose as both a supporting electrolyte and brominating agent. The method offers a broad substrate scope, high atom economy, and excellent diastereoselectivity. The stereoselectivity of the product is controlled by minimizing the dipolar repulsion between the amide C=O and the C-Br bonds. We also explored the methodology's versatility by applying it to various functionalizations and demonstrated its scalability for practical use. The efficient derivatization of the products allowed for the rapid creation of a diverse library of functionalized spirocyclobutyl oxindoles.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401701"},"PeriodicalIF":7.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142491601","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 : 2024-10-21DOI: 10.1002/cssc.202400444
Roger de Paz-Castany, Konrad Eiler, Aliona Nicolenco, Maria Lekka, Eva García-Lecina, Guillaume Brunin, Gian-Marco Rignanese, David Waroquiers, Thomas Collet, Annick Hubin, Eva Pellicer
{"title":"Hydrogen Evolution Reaction of Electrodeposited Ni-W Films in Acidic Medium and Performance Optimization Using Machine Learning.","authors":"Roger de Paz-Castany, Konrad Eiler, Aliona Nicolenco, Maria Lekka, Eva García-Lecina, Guillaume Brunin, Gian-Marco Rignanese, David Waroquiers, Thomas Collet, Annick Hubin, Eva Pellicer","doi":"10.1002/cssc.202400444","DOIUrl":"10.1002/cssc.202400444","url":null,"abstract":"<p><p>Ni-W alloy films were electrodeposited from a gluconate aqueous bath at pH=5.0, at varying current densities and temperatures. While there is little to no difference in composition, i. e., all films possess ~12 at.% W, their activity at hydrogen evolution reaction (HER) in acidic medium is greatly influenced by differences in surface morphology. The kinetics of HER in 0.5 M H<sub>2</sub>SO<sub>4</sub> indicates that the best performing film was obtained at a current density of -4.8 mA/cm<sup>2</sup> and 50 °C. The Tafel slopes (b) and the overpotentials at a geometric current density of -10 mA/cm<sup>2</sup> (η<sub>10</sub>) obtained for 200 cycles of linear sweep voltammetry (LSV) from a set of films deposited using different parameters were fed into a machine learning algorithm to predict optimum deposition conditions to minimize b, η<sub>10</sub>, and the degradation of samples over time. The optimum deposition conditions predicted by the machine learning model led to the electrodeposition of Ni-W films with superior performance, exhibiting b of 33-45 mV/dec and an η<sub>10</sub> of 0.09-0.10 V after 200 LSVs.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202400444"},"PeriodicalIF":7.5,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142454147","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 : 2024-10-21DOI: 10.1002/cssc.202401429
Zhenqiang Ge, Hangning Liu, Shan Wang, Yingjun Ma, Wenhao Xu, Linghao Su, Lei Han, Liangyu Gong, Jie Wang
{"title":"Optimizing Aqueous Zinc-Sulfur Battery Performance via Regulating Acetonitrile Co-Solvents and Carbon Nanotube Carriers.","authors":"Zhenqiang Ge, Hangning Liu, Shan Wang, Yingjun Ma, Wenhao Xu, Linghao Su, Lei Han, Liangyu Gong, Jie Wang","doi":"10.1002/cssc.202401429","DOIUrl":"10.1002/cssc.202401429","url":null,"abstract":"<p><p>Rechargeable aqueous zinc-sulfur batteries (AZSBs) are gaining attention due to their high energy density, ultra-stable discharge platform, and safety. However, poor liquid/solid reaction processes at the anode and cathode reduce reaction kinetics, and the severe dissolution of polysulfides causes shuttle effects during discharge/charge cycles, hindering practical applications. Improving performance requires optimizing both the cathode and electrolyte. Herein, we design an organic-inorganic hybrid electrolyte (zinc trifluoromethanesulfonate and trace iodine monomer dissolved in an acetonitrile/water co-solvent (AN-X)) and a partially exfoliated multi-walled carbon nanotube (PECNT) hosted sulfur (S@PECNTs) cathode for AZSBs. The sulfur is highly dispersed along the PECNTs with appropriate wettability at the electrode/electrolyte interface using AN-3 as the electrolyte. Meanwhile, this electrolyte inhibits hydrogen evolution at negative potentials and promotes uniform Zn ion stripping/plating. Expressively, the AN-3-based AZSB exhibits a high discharge capacity of 1370 mAh g<sup>-1</sup> with excellent Coulombic efficiency (79.9 %), outstanding rate capability, and cycling performance. These improvements are attributed to the synergistic effect between the S@PECNTs and the AN-3 electrolyte, which reduces R<sub>ct</sub> to enhance reaction kinetics and blocks the dissolution and shuttle effect of polysulfides, ensuring a reversible reaction between zinc and sulfur.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401429"},"PeriodicalIF":7.5,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142454158","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 : 2024-10-21DOI: 10.1002/cssc.202401699
Rongbin Miao, Qing Niu, Liuyi Li, Yan Yu
{"title":"Ni-Metalized Covalent Organic Cage as a Photocatalyst for Selective Photoreduction of CO<sub>2</sub> to CO.","authors":"Rongbin Miao, Qing Niu, Liuyi Li, Yan Yu","doi":"10.1002/cssc.202401699","DOIUrl":"10.1002/cssc.202401699","url":null,"abstract":"<p><p>Metal complex-based photocatalysts are promising for CO<sub>2</sub> reduction. Their catalytic performances greatly rely on the synergy of ligands and metal ions. Here, we demonstrate an assembly of covalent organic cage (COC) and metal ions for photocatalytic CO<sub>2</sub> reduction. The coordinated metal serves as catalytically active site for CO<sub>2</sub> reduction, while the cage not only chelates the metal site, but also enhances the local concentration of CO<sub>2</sub> around metal site, and decreases the key intermediate reaction energy barrier, thereby promoting the CO<sub>2</sub> reduction reaction kinetically and thermodynamically. Accordingly, a Ni metalized COC exhibited outstanding photocatalytic performance in CO<sub>2</sub>-to-CO conversion under visible light irradiation. This study highlights the feasibility and advantage of organic cages for the construction of photocatalysts for artificial photosynthesis.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401699"},"PeriodicalIF":7.5,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142454155","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}