Frontiers of Chemical Science and Engineering最新文献

{"title":"Mechanistic studies of zeolite catalysis via in situ solid-state nuclear magnetic resonance spectroscopy: progress and prospects","authors":"Chao Wang,&nbsp;Min Hu,&nbsp;Jun Xu,&nbsp;Feng Deng","doi":"10.1007/s11705-024-2505-2","DOIUrl":"10.1007/s11705-024-2505-2","url":null,"abstract":"<div><p>Zeolites, with their exquisite microporous frameworks and tailorable acidities, serve as ubiquitous catalysts across a diverse spectrum of industrial applications, ranging from petroleum and coal processing to sustainable chemistry and environmental remediation. Optimizing their performance hinges on a thorough understanding of the structure-performance relationship. <i>In situ</i> solid-state nuclear magnetic resonance spectroscopy has emerged as a critical tool, providing unparalleled atomic-level insights into both structure and dynamic aspects of zeolite-catalyzed reactions. Herein, we review recent progress in the development and application of the <i>in situ</i> solid-state nuclear magnetic resonance technique to zeolite catalysis. We first review the <i>in situ</i> nuclear magnetic resonance techniques used in zeolite-catalyzed reaction, including batch-like and continuous-flow reaction modes. The conditions and limitations for these techniques are thoroughly summarized. Subsequently, we review the applications of <i>in situ</i> nuclear magnetic resonance techniques in zeolite-catalyzed reaction, focusing on some important catalytic reactions like methanol-to-hydrocarbons, ethanol dehydration, alkane activation, and beyond. Emphasis is placed on the strategies of specific <i>in situ</i> nuclear magnetic resonance methodologies to tackle critical challenges encountered in these fields, such as probing intermediates and unraveling reaction mechanisms. Additionally, we discuss the burgeoning opportunities and prospective challenges associated with <i>in situ</i> nuclear magnetic resonance studies of zeolite-catalyzed processes.\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":"19 1","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691963","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":"Excellent charge separation over NiCo2S4/CoTiO3 nanocomposites improved photocatalytic hydrogen production","authors":"Linlin Fan,&nbsp;Xin Guo,&nbsp;Lujun Wang,&nbsp;Zhiliang Jin,&nbsp;Noritatsu Tsubaki","doi":"10.1007/s11705-024-2509-y","DOIUrl":"10.1007/s11705-024-2509-y","url":null,"abstract":"<div><p>The rapid migration and separation of photoinduced carriers is a key factor influencing photocatalytic efficiency. Constructing an S-scheme heterojunction is a strategic technique to enhance the separation of photo-generated carriers and boost overall catalytic activity. Herein, a simple physical stirring technique was adopted to successfully fabricate a novel NiCo₂S₄/CoTiO₃ S-scheme heterojunction photocatalyst. Upon exposure to light, the NiCo₂S₄/CoTiO₃-10 specimen demonstrated an outstanding hydrogen evolution rate of 2037.76 µmol·g⁻¹·h⁻¹, exceeding twice the rate observed for the pristine NiCo₂S₄ (833.72 µmol·g⁻¹·h⁻¹). The experimental outcomes reveal that the incorporation of CoTiO₃ significantly enhances the charge separation and transfer within the system. Concurrently, the formation of the S-scheme mechanism facilitates the separation of carriers while maintaining high redox capabilities. This work introduces an innovative approach to forming S-scheme heterojunctions based on bimetallic sulfides, thereby offering new prospects for the efficient utilization of solar energy.</p></div>","PeriodicalId":571,"journal":{"name":"Frontiers of Chemical Science and Engineering","volume":"19 1","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691843","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":"What makes biochar an interesting CO2 adsorbent?","authors":"Antony Rajendran,&nbsp;Arumugam Sakthivel,&nbsp;Zhiwei Dong,&nbsp;Wenying Li","doi":"10.1007/s11705-024-2516-z","DOIUrl":"10.1007/s11705-024-2516-z","url":null,"abstract":"<div><p>Biochar belongs to the category of low-cost, stable, and environmentally benign carbon-based materials. In this article, the reasons that highlight the advantages of biochar materials to be used in carbon dioxide (CO₂) adsorption are briefly viewed with recent examples. Also, the issues to be solved for recommending biochar materials in the practical applications are listed.\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":"19 2","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142761892","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":"Probing the dynamics of methanol in copper-loaded zeolites via quasi-elastic and inelastic neutron scattering","authors":"Vainius Skukauskas,&nbsp;Nicolas De Souza,&nbsp;Emma K. Gibson,&nbsp;Ian P. Silverwood","doi":"10.1007/s11705-024-2506-1","DOIUrl":"10.1007/s11705-024-2506-1","url":null,"abstract":"<div><p>The dynamics of methanol within prototype methanol synthesis catalysts were studied using quasi-elastic neutron scattering. Three Cu-exchanged zeolites (mordenite, SSZ-13 and ZSM-5) were studied after methanol loading and showed jump diffusion coefficients between 1.04 × 10⁻¹⁰ and 2.59 × 10⁻¹⁰ m²·s⁻¹. Non-Arrhenius behavior was observed with varying temperature due to methoxy formation at Brønsted acid sites and methanol clustering around copper cations.\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":"19 1","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691845","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":"Effective lateral dispersion of momentum, heat and mass in bubbling fluidized beds","authors":"Gabriel Gustafsson,&nbsp;Guillermo Martinez Castilla,&nbsp;David Pallarès,&nbsp;Henrik Ström","doi":"10.1007/s11705-024-2503-4","DOIUrl":"10.1007/s11705-024-2503-4","url":null,"abstract":"<div><p>The lateral dispersion of bed material in a bubbling fluidized bed is a key parameter in the prediction of the effective in-bed heat transfer and transport of heterogenous reactants, properties important for the successful design and scale-up of thermal and/or chemical processes. Computational fluid dynamics simulations offer means to investigate such beds in silico and derive effective parameters for reduced-order models. In this work, we use the Eulerian-Eulerian two-fluid model with the kinetic theory of granular flow to perform numerical simulations of solids mixing and heat transfer in bubbling fluidized beds. We extract the lateral solids dispersion coefficient using four different methods: by fitting the transient response of the bed to (1) an ideal heat or (2) mass transfer problem, (3) by extracting the time-averaged heat transfer behavior and (4) through a momentum transfer approach in an analogy with single-phase turbulence. The method (2) fitting against a mass transfer problem is found to produce robust results at a reasonable computational cost when assessed against experiments. Furthermore, the gas inlet boundary condition is shown to have a significant effect on the prediction, indicating a need to account for nozzle characteristics when simulating industrial cases.\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 12","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11705-024-2503-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142412716","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Recent progress in the interfacial polymerization process for CO2 separation membrane fabrication","authors":"Zhijie Shang,&nbsp;Qiangqiang Song,&nbsp;Bin Han,&nbsp;Jing Ma,&nbsp;Dongyang Li,&nbsp;Cancan Zhang,&nbsp;Xin Li,&nbsp;Jinghe Yang,&nbsp;Junyong Zhu,&nbsp;Wenpeng Li,&nbsp;Jing Wang,&nbsp;Yatao Zhang","doi":"10.1007/s11705-024-2510-5","DOIUrl":"10.1007/s11705-024-2510-5","url":null,"abstract":"<div><p>Nowadays, global warming caused by the increasing levels of CO₂ has become a serious environmental problem. Membrane separation technology has demonstrated its promising potential in carbon capture due to its easy operation, energy-efficientness and high efficiency. Interfacial polymerization process, as a facile and well-established technique for preparing membranes with a thin selective layer, has been widely used for fabricating commercial reverse osmosis and nanofiltration membranes in water treatment domain. To push forward such an interfacial polymerization process in the research of CO₂ separation membranes, herein we make a review on the regulation and research progress of the interfacial polymerization membranes for CO₂ separation. First, a comprehensive and critical review of the progress in the monomers, nanoparticles and interfacial polymerization process optimization for preparing CO₂ separation membrane is presented. In addition, the potential of molecular dynamics simulation and machine learning in accelerating the screen and design of interfacial polymerization membranes for CO₂ separation are outlined. Finally, the possible challenges and development prospects of CO₂ separation membranes by interfacial polymerization process are proposed. It is believed that this review can offer valuable insights and guidance for the future advancement of interfacial polymerization membranes for CO₂ separation, thereby fostering its development.</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":"19 1","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691844","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":"Reversible heat-set four-phase transitions of gel1-to-sol1-to-gel2-to-sol2 in binary hydrogels","authors":"Mengjiao Liang,&nbsp;Wenwen Cao,&nbsp;Yaodong Huang","doi":"10.1007/s11705-024-2501-6","DOIUrl":"10.1007/s11705-024-2501-6","url":null,"abstract":"<div><p>A class of supramolecular binary hydrogels is formed from dodecylamine or tridecylamine and sparing carboxylic acids (with amine/acid molar ratio ⩾ 18). These hydrogels exhibit a remarkable thermally reversible four-phase transition. On heating, they transition from gel one (G¹)-to-sol one (Sol¹), then to gel two (G²)-to-sol two (Sol²). On cooling, they revert from Sol²-to-G²-to-Sol¹-to-G¹. Additionally, several G¹ and G² hydrogels undergo thermally reversible gel-to-gel phase transitions, which are reflected by translucent-opaque and opaque-translucent changes in their appearance. The nature of the four-phase transformation was analyzed using a range of techniques. Scanning electron microscopy images confirmed that the fibers of the opaque hydrogel at high temperatures were considerably larger than those of its translucent counterpart at low temperatures. Fluorescence emission spectra demonstrated that higher temperatures, higher amine/acid ratios, and greater acid hydrophobicity increased the hydrophobic interactions. Fourier transform infrared spectroscopy and ultraviolet-visible spectroscopic analyses confirmed the existence of hydrogen-bonding interactions and aggregation in the hydrogels. X-ray diffraction profiles indicated that the hydrogels adopt lamellar structures. The findings advance our current understanding of the phase transition of supramolecular gels and facilitate the constitution of binary or multicomponent gels, providing a practical way to create new smart functional materials.</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 12","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142412523","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":"Synergistic technologies for a circular economy: upcycling waste plastics and biomass","authors":"Ahmed I. Osman,&nbsp;Mahmoud Nasr,&nbsp;Chukwunonso O. Aniagor,&nbsp;Mohamed Farghali,&nbsp;Mee Mee Huang,&nbsp;Bridgid Lai Fui Chin,&nbsp;Ziqiang Sun,&nbsp;Serene Sow Mun Lock,&nbsp;Eduardo A. López-Maldonado,&nbsp;Chung Loong Yiin,&nbsp;Charles E. Chinyelu,&nbsp;Abid Salam Farooqi,&nbsp;Zhonghao Chen,&nbsp;Pow-Seng Yap","doi":"10.1007/s11705-024-2507-0","DOIUrl":"10.1007/s11705-024-2507-0","url":null,"abstract":"<div><p>The urgent need for sustainable waste management has led to the exploration of upcycling waste plastics and biomass as viable solutions. In 2018, global plastic production reached 359 million tonnes, with an estimated 12000 million tonnes projected to be delivered and disposed of in landfills by 2050. Unfortunately, current waste management practices result in only 19.5% of plastics being recycled, while the rest is either landfilled (55%) or incinerated (25.5%). The improper disposal of plastics contributes to issues such as soil and groundwater contamination, air pollution, and wildlife disturbance. On the other hand, biomass has the potential to deliver around 240 exajoules of energy per year by 2060. However, its current utilization remains relatively small, with only approximately 9% of biomass-derived energy being consumed in Europe in 2017. This review explores various upcycling methods for waste plastics and biomass, including mechanical, chemical, biological, and thermal approaches. It also highlights the applications of upcycled plastics and biomass in sectors such as construction, packaging, energy generation, and chemicals. The environmental and economic benefits of upcycling are emphasized, including the reduction of plastic pollution, preservation of natural resources, carbon footprint reduction, and circular economy advancement.\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":"19 1","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s11705-024-2507-0.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691970","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhanced C3H6/C3H8 separation performance in polysulfone membrane blended with rigid ZIF-8 crystals","authors":"Jiayu Luo,&nbsp;Luxi Lyu,&nbsp;Zongjie Yin,&nbsp;Yanying Wei","doi":"10.1007/s11705-024-2504-3","DOIUrl":"10.1007/s11705-024-2504-3","url":null,"abstract":"<div><p>Metal-organic frameworks have a wide range of applications in the field of membrane separation, but the inherent flexible structure and the difficulty for scale-up hinder their further applications. Herein, the relatively rigid zeolitic imidazolate framework-8 particles prepared under an electric field (E-ZIF-8) were used as the fillers in polysulfone (PSF) to form series of mixed matrix membranes. It was found that the introduction of E-ZIF-8 improves both the C₃H₆ permeability and C₃H₆/C₃H₈ selectivity of the membranes. Compared with the bare PSF membrane, the C₃H₆/C₃H₈ selectivity of the 30 wt % E-ZIF-8@PSF membrane increased by ∼230%, while the C₃H₆ permeability was enhanced by ∼830%. In addition, time and pressure dependence analysis demonstrated that such E-ZIF-8@PSF membranes also exhibited good long-term stability and pressure resistance, offering significant industrialization advantages.\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":"19 1","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691971","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":"Investigating CO2 electro-reduction mechanisms: DFT insight into earth-abundant Mn diimine catalysts for CO2 conversions over hydrogen evolution reaction, feasibility, and selectivity considerations","authors":"Murugesan Panneerselvam,&nbsp;Marcelo Albuquerque,&nbsp;Iuri Soter Viana Segtovich,&nbsp;Frederico W. Tavares,&nbsp;Luciano T. Costa","doi":"10.1007/s11705-024-2502-5","DOIUrl":"10.1007/s11705-024-2502-5","url":null,"abstract":"<div><p>This study investigates the detailed mechanism of CO₂ conversion to CO using the manganese(I) diimine electrocatalyst [Mn(pyrox)(CO)₃Br], synthesized by Christoph Steinlechner and coworkers. Employing density functional theory calculations, we thoroughly explore the electrocatalytic pathway of CO₂ reduction alongside the competing hydrogen evolution reaction. Our analysis reveals the significant role of diimine nitrogen coordination in enhancing the electron density of the Mn center, thereby favoring both CO₂ reduction and hydrogen evolution reaction thermodynamically. Furthermore, we observe that triethanolamine (TEOA) stabilizes transition states, aiding in CO₂ fixation and reduction. The critical steps influencing the reaction rate involve breaking the MnC(O)–OH bond during CO₂ reduction and cleaving the MnH–H–TEOA bond in the hydrogen evolution reaction. We explain the preference for CO₂ conversion to CO over H₂ evolution due to the higher energy barrier in forming the Mn-H₂ species during H₂ production. Our findings suggest the potential for tuning the electron density of the Mn center to enhance reactivity and selectivity in CO₂ reduction. Additionally, we analyze potential competing reactions, focusing on electrocatalytic processes for CO₂ reduction and evaluating “protonation-first” and “reduction-first” pathways through density functional theory calculations of redox potentials and Gibbs free energies. This analysis indicates the predominance of the “reduction-first” pathway in CO production, especially under high applied potential conditions. Moreover, our research highlights the selectivity of [Mn(pyrox)(CO)₃Br] toward CO production over HCOO⁻ and H₂ formation, proposing avenues for future research to expand upon these findings by using larger basis sets and exploring additional functionalized ligands.</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 12","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142411611","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}