ACS Sustainable Chemistry & Engineering最新文献

Temperature-Programmed Alkaline Thermal Treatment of Lignocellulosic Biomass to Produce Fractionated Hydrogen with High Production Capacity

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2024-06-26 DOI: 10.1021/acssuschemeng.4c02652

Guojie Liu, Houfang Lu, Xingyu Gong, Kejing Wu, Guoqing Guan, Bin Liang

{"title":"Temperature-Programmed Alkaline Thermal Treatment of Lignocellulosic Biomass to Produce Fractionated Hydrogen with High Production Capacity","authors":"Guojie Liu, Houfang Lu, Xingyu Gong, Kejing Wu, Guoqing Guan, Bin Liang","doi":"10.1021/acssuschemeng.4c02652","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c02652","url":null,"abstract":"H2 production is severely limited by inefficient conversion of feedstock, inevitable char formation, and methanation reactions aggravated by the slow heating rate during conventional alkaline thermal treatment (ATT) of biomass. Herein, a temperature-programmed alkaline thermal treatment (TP-ATT) incorporating dehydrogenation below 250 °C and rapid alkalinization at 600 °C is developed to produce fractionated H2 with a high production capacity of 46.06 mmol·g–1 of cellulose. The H2 produced via NaOH-promoted dehydrogenation exhibits a high purity of 98%. Optimized TP-ATT achieves complete conversions of cellulose and hemicellulose, and the H2 productions are 46, 24, and 89% higher than those of conventional ATT from cellulose, hemicellulose, and lignin, respectively. Fast heating and steam-promoted alkalinization reactions are essential for the efficient conversion of char with high H2 production. TP-ATT of cellulose realizes a 98.14% energy recovery of both H2 and CH4. The TP-ATT technology is applicable to different real biomass with approximately 43% higher H2 production than conventional ATT.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141461562","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Low Concentration Template Preparation of Microsized Au/TS-1 as an Efficient Catalyst for Gas-Phase Propylene Epoxidation with H2 and O2

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2024-06-26 DOI: 10.1021/acssuschemeng.4c01941

Leilei Hou, Liping Liu, Jiaxu Liu, Guang Xiong

引用次数: 0

TBA(FeCl3Br) Complex as a Photocatalyst in the Csp3–H Bond Activation in Alcohols for the Synthesis of N-Based Heterocycles TBA(FeCl3Br) 复合物作为光催化剂活化醇中的 Csp3-H 键以合成 N 基杂环化合物

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2024-06-25 DOI: 10.1021/acssuschemeng.4c03149

Luiz H. Dapper, Viviane T. Mena, Mateus W. Rambo, Felipe B. Santos, Nahum R. Pineda, Bernardo A. Iglesias, Paulo C. Piquini, Márcio S. Silva, Eder J. Lenardão, Filipe Penteado

引用次数: 0

Eco-Friendly Electrospun Nanofibers Based on Plant Proteins as Tunable and Sustainable Biomaterials 基于植物蛋白的生态友好型电纺纳米纤维--可调节、可持续的生物材料

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2024-06-25 DOI: 10.1021/acssuschemeng.4c00895

Kleopatra Kalouta, Mai Bay Stie, Xuedan Sun, Vito Foderà, Valeria Vetri

{"title":"Eco-Friendly Electrospun Nanofibers Based on Plant Proteins as Tunable and Sustainable Biomaterials","authors":"Kleopatra Kalouta, Mai Bay Stie, Xuedan Sun, Vito Foderà, Valeria Vetri","doi":"10.1021/acssuschemeng.4c00895","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c00895","url":null,"abstract":"Plant protein-based nanofibers generated by eco-friendly waterborne electrospinning are emerging as sustainable and innovative materials with vast applications in different biomedical areas. In this study, we fabricated electrospun nanofibers based on potato, pea, and soy protein isolates, achieving remarkably high protein content without the use of organic solvents, strong bases, or surfactants. The different protein nanofibers were characterized by means of quantitative fluorescence imaging, optical spectroscopy, and dynamic mechanical analysis. Results indicated that the intrinsic nature of the proteins modulated the properties of the nanofibers in terms of morphology, fluorescence fingerprints, mechanical strength, and stability in aqueous environments. Pea and soy protein isolates, both rich in β-structure, led to the formation of robust and dense nanofibers, which slowly disintegrated in water. On the contrary, less dense and highly soluble nanofibers were generated from the structurally more flexible potato protein isolate, and these nanofibers demonstrated lower resistance to breakage. Our findings indicate the importance of protein structural elements when designing protein-based electrospun nanofibers with specific features. Deciphering the intricate relationship between protein structure at the molecular level and properties of nanofiber holds promise for the development of biomaterials with enhanced efficacy in diverse biomedical applications.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453284","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Selective Multifunctional Aliphatic Amine Synthesis: Unraveling Universal Control Strategies in Catalytic Reductive Amination of Biobased α-Hydroxy Carbonyl Oxygenates 选择性多功能脂肪胺合成：揭示生物基 α-羟基羰氧化合物催化还原胺化过程中的通用控制策略

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2024-06-25 DOI: 10.1021/acssuschemeng.4c02649

Benjamin Vermeeren, Sofie Van Praet, Axelle De Ridder, Bert F. Sels

{"title":"Selective Multifunctional Aliphatic Amine Synthesis: Unraveling Universal Control Strategies in Catalytic Reductive Amination of Biobased α-Hydroxy Carbonyl Oxygenates","authors":"Benjamin Vermeeren, Sofie Van Praet, Axelle De Ridder, Bert F. Sels","doi":"10.1021/acssuschemeng.4c02649","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c02649","url":null,"abstract":"Catalytic reductive amination of carbohydrate-derived α-hydroxy carbonyl oxygenates offers an elegant approach to access both aliphatic alkanolamines and alkyl polyamines via the same reaction pathway. However, the advantage of producing these distinct aliphatic amine products from a single feedstock is accompanied by the challenge of product selectivity. This work therefore focused on exploring asymmetrically substituted α-hydroxy carbonyl oxygenates as an uncharted, yet potentially valuable subgroup of substrates. Here, the selectivity challenge was tackled by comprehensively assessing the effectiveness of multiple control handles based on the underlying reaction mechanism. These handles ranged from reaction parameters such as (co-)catalyst selection, reaction temperature, amine-to-substrate molar ratio, and solvent choice to process design, encompassing one-step and one-pot-two-step approaches. By synergistically combining the most decisive handles, we distilled three distinct, universally applicable and highly selective control strategies. Each strategy was tailored to regulate the formation of either one of the two alkanolamine isomers or the polyamine product. As a proof of concept, a strategy was proposed, inspired by the polyamine-tailored strategy, favoring the formation of high-value asymmetrically substituted alkyl polyamines. This proof of concept underscored the importance of both the relative reactivity of the two amine reactants and the stability of the formed α-amino ketone intermediate.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453223","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Facile Fabrication of High-Power Molybdenum Diselenide Cathode for Rechargeable Magnesium Batteries 轻松制备用于可充电镁电池的大功率二硒化钼阴极

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2024-06-25 DOI: 10.1021/acssuschemeng.4c03206

Donggang Tao, Yudi Tang, Hongda Gui, Fei Xu

{"title":"Facile Fabrication of High-Power Molybdenum Diselenide Cathode for Rechargeable Magnesium Batteries","authors":"Donggang Tao, Yudi Tang, Hongda Gui, Fei Xu","doi":"10.1021/acssuschemeng.4c03206","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c03206","url":null,"abstract":"Rechargeable magnesium batteries are favorable for grid energy storage, but the lack and low performance of the cathodes is hindering the development. 2D-layered transition metal dichalcogenides based on Ti, V, Mo, and W would be promising selections due to the high covalent bond content enhancing charge delocalization and structure stability. Specifically, the 1T phase is more advantageous than the 2H phase for magnesium storage because of the high conductivity and large interlayer spacing, but the fabrication is quite difficult due to the thermodynamic instability. Herein, a simple method is developed to fabricate molybdenum diselenide with high 1T phase content, using hydrazine hydrate to generate electron donating N-containing components coordinating with Mo and facilitating the formation of the 1T phase. The synthesized molybdenum diselenide shows a high capacity of 180 mA h g–1 at 50 mA g–1 and an outstanding kinetic performance of 93 mA h g–1 at 5 A g–1. A mechanism study indicates that magnesium storage could be defined as an intercalation reaction. The larger interlayer spacing of 1T phase improves the Mg2+ diffusion and enhances the kinetic performance at high current densities. The present study delivers insights into the fabrication of high-performance transition metal dichalcogenide cathode materials for RMBs.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453273","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Efficient Self-Condensation of Cyclohexanone into Biojet Fuel Precursors over Sulfonic Acid-Modified Silicas: Insights on the Effect of Pore Size and Structure 在磺酸改性硅胶上将环己酮高效自缩合为生物喷气燃料前体：洞察孔径和结构的影响

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2024-06-24 DOI: 10.1021/acssuschemeng.4c01956

Antonio Martín, Esther Arribas-Yuste, Marta Paniagua, Gabriel Morales, Juan A. Melero

{"title":"Efficient Self-Condensation of Cyclohexanone into Biojet Fuel Precursors over Sulfonic Acid-Modified Silicas: Insights on the Effect of Pore Size and Structure","authors":"Antonio Martín, Esther Arribas-Yuste, Marta Paniagua, Gabriel Morales, Juan A. Melero","doi":"10.1021/acssuschemeng.4c01956","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c01956","url":null,"abstract":"Mesoporous silica materials with different pore structures and sizes have been used for supporting aryl sulfonic acid catalytic sites via a postsynthetic grafting approach. The synthesized materials have been evaluated in the solventless acid-catalyzed self-condensation of cyclohexanone (CHO) to obtain the corresponding C12 adducts. These compounds display great potential as oxygenated fuel precursors as they can be transformed into jet fuel range alkanes in a subsequent hydrodeoxygenation process. In this work, the synthesized catalysts have displayed high selectivity values toward monocondensed compounds (>95%), thus limiting the formation of undesired heavier condensation products, together with CHO conversion values in the range 20–40% after 2 h of reaction at 100 °C. The structural and textural properties of the supports play an important role in the catalytic performance. Moreover, the activity per acid center is correlated with the textural properties of the supports, indicating that a lower surface density of the anchored aryl sulfonic groups affords an improvement in their specific activity. Finally, the benefit of using supports with large pore sizes and open structures, which limit the fouling of the catalysts by organic deposits, is demonstrated in a stability and reusability test.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453214","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Solvent-Free Carboxylative Cyclization of CO2 with Alkynol Catalyzed by Ag(I)-Functionalized Polyoxoniobate-Based Coordination Polymer at Room Temperature Ag(I)-Functionalized Polyoxoniobate-Based Coordination Polymer 在室温下催化 CO2 与炔醇的无溶剂羧基环化反应

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2024-06-24 DOI: 10.1021/acssuschemeng.4c02727

Zouguang Han, Hongrui Tian, Jiaqi Qin, Weina Cai, Baokuan Chen, Yanfeng Bi

{"title":"Solvent-Free Carboxylative Cyclization of CO2 with Alkynol Catalyzed by Ag(I)-Functionalized Polyoxoniobate-Based Coordination Polymer at Room Temperature","authors":"Zouguang Han, Hongrui Tian, Jiaqi Qin, Weina Cai, Baokuan Chen, Yanfeng Bi","doi":"10.1021/acssuschemeng.4c02727","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c02727","url":null,"abstract":"Transforming gaseous waste CO2 as a C1 feedstock into fine chemicals is significant for green chemistry and sustainable development. Herein, the novel Ag(I)-functionalized polyoxoniobate-based coordination polymer {[Ag(tpy)]5[Nb10O28]}[Ag(H2O)]·5H2O (1, tpy = 2,2′:6′,2″-terpyridine) is successfully fabricated and fully characterized. Compound 1 not only displays excellent thermal and solvent stabilities but can also efficiently and selectively catalyze the solvent-free carboxylative cyclization of terminal propargylic alcohols with different substituents with CO2 to high-value-added α-alkylidene cyclic carbonates at room temperature. The prominent performance of 1 is attributed to the synergistic operation of Ag(I) and [Nb10O28] in its structure, which is responsible for activating the C≡C bond and hydroxyl group of propargylic alcohols, respectively. The catalyst exhibits outstanding sustainability; no obvious decrease in catalytic activity is observed during five successive cycles, and the yield of α-alkylidene cyclic carbonate in the gram-scale (100 mmol, 8.4 g) experiment is up to 61.7% (turnover number value = 5144). To the best of our knowledge, this represents the first example of polyoxometalate-based catalyst for catalyzing the solvent-free conversion of CO2 to value-added chemicals at room temperature.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453272","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Investigation of Carbonation Kinetics in Carbonated Cementitious Materials by Reactive Molecular Dynamics Simulations 通过反应分子动力学模拟研究碳化胶凝材料的碳化动力学

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2024-06-24 DOI: 10.1021/acssuschemeng.3c07814

Ling Qin, Qijie Xie, Jiuwen Bao, Gaurav Sant, Tiefeng Chen, Peng Zhang, Ditao Niu, Xiaojian Gao, Mathieu Bauchy

{"title":"Investigation of Carbonation Kinetics in Carbonated Cementitious Materials by Reactive Molecular Dynamics Simulations","authors":"Ling Qin, Qijie Xie, Jiuwen Bao, Gaurav Sant, Tiefeng Chen, Peng Zhang, Ditao Niu, Xiaojian Gao, Mathieu Bauchy","doi":"10.1021/acssuschemeng.3c07814","DOIUrl":"https://doi.org/10.1021/acssuschemeng.3c07814","url":null,"abstract":"Calcium carbonate (CaCO3) precipitation plays a significant role during the carbon capture process; however, the mechanism is still only partially understood. Understanding the atomic-level carbonation mechanism of cementitious materials can promote the mineralization capture, immobilization, and utilization of carbon dioxide, as well as the improvement of carbonated cementitious materials’ performance. Therefore, based on molecular dynamics simulations, this paper investigates the effect of Si/Al concentrations in cementitious materials on carbonation kinetics. We first verify the force field used in this paper. Then, we analyze the network connectivity evolution, the number and size of the carbonate cluster during gelation, the polymerization rate, and the activation energy. Finally, in order to reveal the reasons that caused the evolution of polymerization rate and activation energy, we analyze the local stress and charge of atoms. Results show that the Ca–Oc bond number and carbonate cluster size increase with the decrease of the Si/Al concentration and the increase of temperature, leading to the higher amorphous calcium carbonate gel polymerization degree. The local stress of each atom in the system is the driving force of the gelation transition. The presence of Si and Al components increases the atom’s local stress and average charge, thus causing the increase of the energy barrier of CaCO3 polymerization and the activation energy of carbonation.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141453192","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Chemo-enzymatic Synthesis of Coenzyme A Using Copurified Enzymes from Probiotic Escherichia coli Nissle

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2024-06-24 DOI: 10.1021/acssuschemeng.4c03510

Wan-Wen Ting, Shota Nishikawa, Wen-Chi Yu, Ming-Jing He, Hui-Chun Chen, Kosuke Fujishima, Yi-Jung Sung, Kai-Cheng Wang, I-Son Ng, Po-Hsiang Wang

{"title":"Chemo-enzymatic Synthesis of Coenzyme A Using Copurified Enzymes from Probiotic Escherichia coli Nissle","authors":"Wan-Wen Ting, Shota Nishikawa, Wen-Chi Yu, Ming-Jing He, Hui-Chun Chen, Kosuke Fujishima, Yi-Jung Sung, Kai-Cheng Wang, I-Son Ng, Po-Hsiang Wang","doi":"10.1021/acssuschemeng.4c03510","DOIUrl":"https://doi.org/10.1021/acssuschemeng.4c03510","url":null,"abstract":"Coenzyme A (CoA) is an indispensable cofactor carrying fundamental building blocks in cells (e.g., acetyl-CoA). However, in vivo CoA synthesis is often limited by feedback inhibition and the cost of purification; instead, in vitro enzymatic CoA synthesis represents a sustainable alternative. Herein, we present a one-pot chemo-enzymatic cascade pathway for free CoA synthesis from pantethine using recombinant enzymes purified from probiotic Escherichia coli Nissle (endotoxin-free), along with the polyphosphate kinase system for ATP regeneration and the phosphite dehydrogenase system for NADH regeneration, respectively. First, we selected the nontoxic biological reductant glutathione for chemical pantethine reduction, where the glutathione is readily reduced by the NAD(P)H-dependent glutathione reductase. The one-pot enzymatic cascade (comprising pantothenate kinase, pantetheine-phosphate adenylyltransferase, and dephospho-CoA kinase) then completely converts pantetheine into free CoA in 2 h with a titer of ∼2 mM (1.5 g/L) in a 0.1 mL reaction system. Finally, the quality of the chemoenzymatically synthesized CoA rivals that of the commercial CoA standard for acetyl-CoA synthesis. Copurifying the recombinant enzymes from probiotic E. coli Nissle and the use of inorganic phosphate buffer further reduce the environmental burdens and carbon footprint of the whole process. Therefore, the present work could serve as a paradigm for future industrial production of acyl-CoA derivatives and other valuable cofactors.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141461718","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0