Frontiers of Chemical Science and Engineering最新文献

{"title":"Single-atom catalysis: a promising avenue for precisely controlling reaction pathways","authors":"Xiaobo Yang,&nbsp;Xuning Li,&nbsp;Yanqiang Huang","doi":"10.1007/s11705-024-2434-0","DOIUrl":"10.1007/s11705-024-2434-0","url":null,"abstract":"<div><p>Single-atom catalysts (SACs), characterized by exceptionally high atom efficiency, have garnered significant attention across various catalytic reactions. Recent studies have showcased SACs with robust capabilities for precise catalysis, specifically targeting reactions along designated pathways. This review focuses on the advances in the precise activation and reconstruction of chemical bonds on SACs, including precise activation of C–O and C–H bonds and selective couplings involving C–C and C–N bonds. Our discussion begins with a thorough exploration of the factors that render SACs skilled in precise catalytic processes, encompassing the narrow <i>d</i>-band electronic state of single atom site resulting in the adsorption tendency, isolate site resulting in unique adsorption structure, and synergy effect of a single atom site with its neighbors. Subsequently, we elaborate on the applications of SACs in electrocatalysis and thermocatalysis including four prominent reactions, namely, electrochemical CO₂ reduction, urea electrochemical synthesis, CO₂ hydrogenation, and CH₄ activation. Then the concept of rational design of SACs for precisely controlling reaction pathways is discussed from the aspects of pore structure design, support-metal strong interaction, and support hydrophilic/hydrophobic. Finally, we summarize the challenges encountered by SACs in the field of precise catalytic processes and outline prospects for their further development in this domain.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"18 7","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-06-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511883","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Deciphering the intermolecular interactions for separating bicyclic and tricyclic aromatics via different naphthalene-based solvents","authors":"Pengzhi Bei,&nbsp;Antony Rajendran,&nbsp;Jie Feng,&nbsp;Wen-Ying Li","doi":"10.1007/s11705-024-2462-9","DOIUrl":"10.1007/s11705-024-2462-9","url":null,"abstract":"<div><p>The traditional separation of bicyclic and tricyclic aromatics from coal tar involves complicated multi-steps and consumes significantly more energy. Previous work accomplished the separation between anthracene-phenanthrene isomers using electrostatic interaction, but for the separation between bicyclic and tricyclic aromatics, electrostatic interactions are difficult to produce a recognizable effect. Naphthalene-based solvents, named as naphthaleneacetamide, naphthaleneethanol, naphthalenemethanol, naphthol, naphthylacetic acid, naphthylacetonitrile, and naphthylamine, respectively, were used for the efficient separation of naphthalene and phenanthrene via dispersion interaction. Results showed that the pre-studied structural parameters are the key factors in selecting an efficient solvent. And the substituents on the intermolecular interactions involved in the separation processes had an important impact, which were evaluated. Naphthalenemethanol exhibited a superior performance with a purity of 96.3 wt % naphthalene products because its electron-donating substituent enables the selective recognition of naphthalene via the dispersion interaction. The used naphthalene-based solvents can be regenerated and recycled via back extraction with a purity of over 90 wt % naphthalene products, suggesting solvent structural stability during the regeneration processes. Notably, the naphthalene-based solvents also demonstrated better separation performance for polycyclic aromatics from coal tar with a purity of over 80 wt % for bicyclic aromatics. This study would enhance the utilization of coal tar as a valuable source of polycyclic aromatics besides broadening the knowledge for applying non-bonded interaction in the separation of polycyclic aromatics technologies.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"18 10","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141347866","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Zeolites for the separation of ethylene, ethane, and ethyne","authors":"Binyu Wang,&nbsp;Qiang Li,&nbsp;Haoyang Zhang,&nbsp;Jia-Nan Zhang,&nbsp;Qinhe Pan,&nbsp;Wenfu Yan","doi":"10.1007/s11705-024-2459-4","DOIUrl":"10.1007/s11705-024-2459-4","url":null,"abstract":"<div><p>The cost-effective separation of ethylene (C₂H₄), ethyne (C₂H₂), and ethane (C₂H₆) poses a significant challenge in the contemporary chemical industry. In contrast to the energy-intensive high-pressure cryogenic distillation process, zeolite-based adsorptive separation offers a low-energy alternative. This review provides a concise overview of recent advancements in the adsorptive separation of C₂H₄, C₂H₂, and C₂H₆ using zeolites or zeolite-based adsorbents. It commences with an examination of the industrial significance of these compounds and the associated separation challenges. Subsequently, it systematically examines the utilization of various types of zeolites with diverse cationic species in such separation processes. And then it explores how different zeolitic structures impact adsorption and separation capabilities, considering principles such as cation-π interaction, π-complexation, and steric separation concerning C₂H₄, C₂H₂, and C₂H₆ molecules. Furthermore, it discusses methods to enhance the separation performance of zeolites and zeolite-based adsorbents, encompassing structural design, modifications, and ion exchange processes. Finally, it summarizes current research trends and future directions, highlighting the potential application value of zeolitic materials in the field of C₂H₄, C₂H₂, and C₂H₆ separation and offering recommendations for further investigation.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"18 9","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511983","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Control of aluminum distribution in ZSM-5 zeolite for enhancement of its catalytic performance for propane aromatization","authors":"Zhao Ma,&nbsp;Dezhi Shi,&nbsp;Sen Wang,&nbsp;Mei Dong,&nbsp;Weibin Fan","doi":"10.1007/s11705-024-2439-8","DOIUrl":"10.1007/s11705-024-2439-8","url":null,"abstract":"<div><p>Regulation of aluminum distribution in zeolite framework is an effective method for improving its catalytic performance for propane aromatization. Herein, we found that recrystallization and post-realuminization of ZSM-5 cannot only create hollow structures to enhance the diffusion ability, but also adjust the content and position of paired aluminum species in its framework. Various characterizations results confirmed that increase of paired aluminum content and inducement of more aluminum atoms sited in the intersection cavity are beneficial to the formation of aromatic products in propane aromatization. As a result, the hollow-structured ZSM-5 zeolite with more paired aluminum (H-200-hollow) showed higher propane conversion and aromatics selectivity than other samples at the same conditions. The catalytic performance of H-200-hollow can be further improved by ion-exchanging with a small amount of Ga(III) species. The propane conversion and aromatics selectivity of Ga-200-hollow reached as high as 95% and 70%, respectively, at 540 °C and 1 atm.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"18 8","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141356082","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Recent advances and practical challenges of high-energy-density flexible lithium-ion batteries","authors":"Guangxiang Zhang,&nbsp;Xin Chen,&nbsp;Yulin Ma,&nbsp;Hua Huo,&nbsp;Pengjian Zuo,&nbsp;Geping Yin,&nbsp;Yunzhi Gao,&nbsp;Chuankai Fu","doi":"10.1007/s11705-024-2444-y","DOIUrl":"10.1007/s11705-024-2444-y","url":null,"abstract":"<div><p>With the rapid iteration and update of wearable flexible devices, high-energy-density flexible lithium-ion batteries are rapidly thriving. Flexibility, energy density, and safety are all important indicators for flexible lithiumion batteries, which can be determined jointly by material selection and structural design. Here, recent progress on high-energy-density electrode materials and flexible structure designs are discussed. Commercialized electrode materials and the next-generation high-energy-density electrode materials are analyzed in detail. The electrolytes with high safety and excellent flexibility are classified and discussed. The strategies to increase the mass loading of active materials on the electrodes by designing the current collector and electrode structure are discussed with keys of representative works. And the novel configuration structures to enhance the flexibility of batteries are displayed. In the end, it is pointed out that it is necessary to quantify the comprehensive performance of flexible lithium-ion batteries and simultaneously enhance the energy density, flexibility, and safety of batteries for the development of the next-generation high-energy-density flexible lithium-ion batteries.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"18 8","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141511887","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Multifunctional carbon materials from rugose rose for energy storage and water purification","authors":"Peng-Hui Li,&nbsp;Hui Zhou,&nbsp;Wen-Juan Wu","doi":"10.1007/s11705-024-2447-8","DOIUrl":"10.1007/s11705-024-2447-8","url":null,"abstract":"<div><p>With the advancement of social process, the resource problem is becoming more prominent, biomass materials come into being, and it is becoming more and more important to explore and prepare efficient and multifunctional biomass materials to alleviate the problems of energy storage and water pollution. In this paper, nitrogen-doped hierarchical porous carbon materials (NRRC) were produced by one-step carbonization of withered rose as raw material and melamine as nitrogen source with KOH-activated porosification. The resulting nitrogen-doped porous carbon material had the most abundant pores and the best microspherical graded pore structure, with a specific surface area of up to 1393 m²·g⁻¹, a pore volume of 0.68 cm³·g⁻¹, and a nitrogen-doped content of 5.52%. Electrochemical tests showed that the maximum specific capacitance of NRRC in the three-electrode system was 346.4 F·g⁻¹ (0.5 A·g⁻¹), which was combined with favorable capacitance retention performance and cycling stability. The NRRC//NRRC symmetric supercapacitors were further assembled, and the maximum energy density of a single device was 23.88 Wh·kg⁻¹, which still maintains excellent capacitance retention and cyclic charging/discharging stability. For example, the capacitance retention rate was always close to 96.27% with almost negligible capacitance loss after 10000 consecutive charge/discharge cycles (current density: 10 A·g⁻¹). Regardless of the three-electrode or two-electrode system, the super capacitive performance of NRRC porous carbon materials was comparable to the electrochemical performance of many reported biomass porous carbon materials, which showed better energy storage advantages and practical application potential. In addition, NRRC porous carbon materials had excellent water purification ability. The dye adsorption test confirmed that NRRC had a high adsorption capacity (491.47 mg·g⁻¹) for methylene blue. This undoubtedly also showed a potential and promising avenue for high value-added utilization of this material.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"18 9","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141530406","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Efficient oxidation of monosaccharides to sugar acids under neutral condition in flow reactors with gold-supported activated carbon catalysts","authors":"Ziqin Gong,&nbsp;Zengyong Li,&nbsp;Xu Zeng,&nbsp;Fengxia Yue,&nbsp;Wu Lan,&nbsp;Chuanfu Liu","doi":"10.1007/s11705-024-2457-6","DOIUrl":"10.1007/s11705-024-2457-6","url":null,"abstract":"<div><p>A significant reaction in the synthesis of biomass-based chemicals is the catalyst-based and targeted oxidation of monosaccharides into valuable sugar acids. In this study, an activated carbon supported gold catalyst was used to oxidize glucose and xylose to gluconic acid and xylonic acid under neutral condition. Optimization of reaction conditions for the catalysts was performed using both a batch reactor and a flow-through reactor. In a batch reactor, the yields of gluconic and xylonic acid reached 93% and 92%, respectively, at 90 °C within 180 min. In a flow reactor, both reactions reached a similar yield at 80 °C with the weight hourly space velocity of 47.1 h⁻¹. The reaction kinetics were explored in the flow reactor. The oxidation of glucose and xylose to gluconic and xylonic acid followed a first-order kinetics and the turnover frequency was 0.195 and 0.161 s⁻¹, respectively. The activation energy was evaluated to be 60.58 and 59.30 kJ·mol⁻¹, respectively. This study presents an environmentally friendly and feasible method for the selective oxidation of monosaccharides using an activated carbon supported gold catalyst, benefiting the high-value application of carbohydrates.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"18 9","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141361856","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synthetic auxotrophs accelerate cell factory development through growth-coupled models","authors":"Liangpo Li,&nbsp;Linwei Yu,&nbsp;Xinxiao Sun,&nbsp;Qipeng Yuan,&nbsp;Xiaolin Shen,&nbsp;Jia Wang","doi":"10.1007/s11705-024-2454-9","DOIUrl":"10.1007/s11705-024-2454-9","url":null,"abstract":"<div><p>The engineering of microbial cell factories for the production of high-value chemicals from renewable resources presents several challenges, including the optimization of key enzymes, pathway fluxes and metabolic networks. Addressing these challenges involves the development of synthetic auxotrophs, a strategy that links cell growth with enzyme properties or biosynthetic pathways. This linkage allows for the improvement of enzyme properties by <i>in vivo</i> directed enzyme evolution, the enhancement of metabolic pathway fluxes under growth pressure, and remodeling of metabolic networks through directed strain evolution. The advantage of employing synthetic auxotrophs lies in the power of growth-coupled selection, which is not only high-throughput but also labor-saving, greatly simplifying the development of both strains and enzymes. Synthetic auxotrophs play a pivotal role in advancing microbial cell factories, offering benefits from enzyme optimization to the manipulation of metabolic networks within single microbes. Furthermore, this strategy extends to coculture systems, enabling collaboration within microbial communities. This review highlights the recently developed applications of synthetic auxotrophs as microbial cell factories, and discusses future perspectives, aiming to provide a practical guide for growth-coupled models to produce value-added chemicals as part of a sustainable biorefinery.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"18 9","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141258644","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhanced bioethanol production from sugarcane bagasse: combination of liquid hot water and deep eutectic solvent pretreatment for optimized enzymatic saccharification","authors":"Xiaoling Xian,&nbsp;Biying Li,&nbsp;Shiyong Feng,&nbsp;Jiale Huang,&nbsp;Xinyuan Fu,&nbsp;Ting Wu,&nbsp;Xiaoqing Lin","doi":"10.1007/s11705-024-2438-9","DOIUrl":"10.1007/s11705-024-2438-9","url":null,"abstract":"<div><p>In the present study, a sustainable pretreatment methodology combining liquid hot water and deep eutectic solvent is proposed for the efficient fractionation of hemicellulose, cellulose, and lignin from sugarcane bagasse, thereby facilitating the comprehensive utilization of both C5 and C6 sugars. The application of this combined pretreatment strategy to sugarcane bagasse led to notable enhancements in enzymatic saccharification and subsequent fermentation. Experiment results demonstrate that liquid hot water-deep eutectic solvent pretreatment yielded 85.05 ± 0.66 g·L⁻¹ of total fermentable sugar (glucose: 60.96 ± 0.21 g·L⁻¹, xylose: 24.09 ± 0.87 g·L⁻¹) through enzymatic saccharification of sugarcane bagasse. Furthermore, fermentation of the pretreated sugarcane bagasse hydrolysate yielded 34.33 ± 3.15 g·L⁻¹ of bioethanol. These findings confirm the effectiveness of liquid hot water-deep eutectic solvent pretreatment in separating lignocellulosic components, thus presenting a sustainable and promising pretreatment method for maximizing the valuable utilization of biomass resources.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"18 8","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141387179","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Interfacing biosynthetic CdS with engineered Rhodopseudomonas palustris for efficient visible light-driven CO2–CH4 conversion","authors":"Yu Zhang,&nbsp;Yulei Qian,&nbsp;Zhenye Tong,&nbsp;Su Yan,&nbsp;Xiaoyu Yong,&nbsp;Yang-Chun Yong,&nbsp;Jun Zhou","doi":"10.1007/s11705-024-2460-y","DOIUrl":"10.1007/s11705-024-2460-y","url":null,"abstract":"<div><p>Engineered photosynthetic bacterium <i>Rhodo-pseudomonas palustris</i> is excellent at one-step CO₂ biomethanation and can use near-infrared light sources, overcoming the limitations of conventional photosynthetic systems. The current study constructed a biohybrid system that deposited CdS nanoparticles on <i>R. palustris</i>. This biohybrid system broadens the capture of sustainable solar energy, achieving a 155 nmol·mL⁻¹ biological CH₄ production under full visible light irradiation, 13.4-fold of that by the pure <i>R. palustris</i>. The transcriptome profiles revealed that gene expression related to photosynthetic electron transfer chain, nitrogenase, nanofilaments, and redox stress defense was activated. Accordingly, we attributed the much-enhanced CO₂ biomethanation in the biohybrid system to the remarkable increase in the intracellular reducing power and the stronger rigidity of the cells assisted by photoexcited electrons from CdS nanoparticles. Our discovery offers insight and a promising strategy for improving the current CO₂–CH₄ biomanufacturing system.\u0000</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"18 10","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141388793","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}