首页 > 最新文献

Annual review of chemical and biomolecular engineering最新文献

英文 中文
Small-Scale Phenomena in Reactive Bubbly Flows: Experiments, Numerical Modeling, and Applications. 反应性气泡流中的小尺度现象:实验、数值模拟和应用。
IF 8.4 2区 工程技术 Q1 Chemical Engineering Pub Date : 2021-06-07 DOI: 10.1146/annurev-chembioeng-092220-100517
Michael Schlüter, Sonja Herres-Pawlis, Ulrich Nieken, Ute Tuttlies, Dieter Bothe

Improving the yield and selectivity of chemical reactions is one of the challenging tasks in paving the way for a more sustainable and climate-friendly economy. For the industrially highly relevant gas-liquid reactions, this can be achieved by tailoring the timescales of mixing to the requirements of the reaction. Although this has long been known for idealized reactors and time- and space-averaged processes, considerable progress has been made recently on the influence of local mixing processes. This progress has become possible through joint research between chemists, mathematicians, and engineers. We present the reaction systems with adjustable kinetics that have been developed, which are easy to handle and analyze. We show examples of how the selectivity of competitive-consecutive reactions can be controlled via local bubble wake structures. This is demonstrated for Taylor bubbles and bubbly flows under technical conditions. Highly resolvednumerical simulations confirm the importance of the bubble wake structure for the performance of a particular chemical reaction and indicate tremendous potential for future process improvements.

提高化学反应的收率和选择性是为更可持续和气候友好型经济铺平道路的一项具有挑战性的任务。对于工业上高度相关的气液反应,这可以通过根据反应的要求调整混合的时间尺度来实现。虽然这早已为理想反应器和时间和空间平均过程所知,但最近在局部混合过程的影响方面取得了相当大的进展。通过化学家、数学家和工程师的共同研究,这一进展成为可能。我们介绍了已开发的具有可调动力学的反应体系,这些反应体系易于处理和分析。我们展示了如何通过局部气泡尾流结构控制竞争性连续反应的选择性的例子。这在技术条件下对泰勒气泡和气泡流进行了论证。高分辨率的数值模拟证实了气泡尾流结构对特定化学反应性能的重要性,并指出了未来工艺改进的巨大潜力。
{"title":"Small-Scale Phenomena in Reactive Bubbly Flows: Experiments, Numerical Modeling, and Applications.","authors":"Michael Schlüter,&nbsp;Sonja Herres-Pawlis,&nbsp;Ulrich Nieken,&nbsp;Ute Tuttlies,&nbsp;Dieter Bothe","doi":"10.1146/annurev-chembioeng-092220-100517","DOIUrl":"https://doi.org/10.1146/annurev-chembioeng-092220-100517","url":null,"abstract":"<p><p>Improving the yield and selectivity of chemical reactions is one of the challenging tasks in paving the way for a more sustainable and climate-friendly economy. For the industrially highly relevant gas-liquid reactions, this can be achieved by tailoring the timescales of mixing to the requirements of the reaction. Although this has long been known for idealized reactors and time- and space-averaged processes, considerable progress has been made recently on the influence of local mixing processes. This progress has become possible through joint research between chemists, mathematicians, and engineers. We present the reaction systems with adjustable kinetics that have been developed, which are easy to handle and analyze. We show examples of how the selectivity of competitive-consecutive reactions can be controlled via local bubble wake structures. This is demonstrated for Taylor bubbles and bubbly flows under technical conditions. Highly resolvednumerical simulations confirm the importance of the bubble wake structure for the performance of a particular chemical reaction and indicate tremendous potential for future process improvements.</p>","PeriodicalId":8234,"journal":{"name":"Annual review of chemical and biomolecular engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2021-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39071349","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 7
Wearable and Implantable Soft Bioelectronics: Device Designs and Material Strategies. 可穿戴与植入式软体生物电子学:装置设计与材料策略。
IF 8.4 2区 工程技术 Q1 Chemical Engineering Pub Date : 2021-06-07 DOI: 10.1146/annurev-chembioeng-101420-024336
Sung-Hyuk Sunwoo, Kyoung-Ho Ha, Sangkyu Lee, Nanshu Lu, Dae-Hyeong Kim

High-performance wearable and implantable devices capable of recording physiological signals and delivering appropriate therapeutics in real time are playing a pivotal role in revolutionizing personalized healthcare. However, the mechanical and biochemical mismatches between rigid, inorganic devices and soft, organic human tissues cause significant trouble, including skin irritation, tissue damage, compromised signal-to-noise ratios, and limited service time. As a result, profuse research efforts have been devoted to overcoming these issues by using flexible and stretchable device designs and soft materials. Here, we summarize recent representative research and technological advances for soft bioelectronics, including conformable and stretchable device designs, various types of soft electronic materials, and surface coating and treatment methods. We also highlight applications of these strategies to emerging soft wearable and implantable devices. We conclude with some current limitations and offer future prospects of this booming field.

高性能可穿戴和植入式设备能够记录生理信号并实时提供适当的治疗,在个性化医疗保健的革命中发挥着关键作用。然而,刚性、无机器件和柔软、有机人体组织之间的机械和生化不匹配会造成严重的麻烦,包括皮肤刺激、组织损伤、信噪比受损和服务时间有限。因此,大量的研究工作一直致力于通过使用柔性和可拉伸的设备设计和软材料来克服这些问题。在这里,我们总结了最近软体生物电子学的代表性研究和技术进展,包括符合和可拉伸的器件设计,各种类型的软体电子材料,以及表面涂层和处理方法。我们还重点介绍了这些策略在新兴软可穿戴和植入式设备中的应用。最后,我们总结了目前的一些局限性,并对这一蓬勃发展的领域提出了未来的展望。
{"title":"Wearable and Implantable Soft Bioelectronics: Device Designs and Material Strategies.","authors":"Sung-Hyuk Sunwoo,&nbsp;Kyoung-Ho Ha,&nbsp;Sangkyu Lee,&nbsp;Nanshu Lu,&nbsp;Dae-Hyeong Kim","doi":"10.1146/annurev-chembioeng-101420-024336","DOIUrl":"https://doi.org/10.1146/annurev-chembioeng-101420-024336","url":null,"abstract":"<p><p>High-performance wearable and implantable devices capable of recording physiological signals and delivering appropriate therapeutics in real time are playing a pivotal role in revolutionizing personalized healthcare. However, the mechanical and biochemical mismatches between rigid, inorganic devices and soft, organic human tissues cause significant trouble, including skin irritation, tissue damage, compromised signal-to-noise ratios, and limited service time. As a result, profuse research efforts have been devoted to overcoming these issues by using flexible and stretchable device designs and soft materials. Here, we summarize recent representative research and technological advances for soft bioelectronics, including conformable and stretchable device designs, various types of soft electronic materials, and surface coating and treatment methods. We also highlight applications of these strategies to emerging soft wearable and implantable devices. We conclude with some current limitations and offer future prospects of this booming field.</p>","PeriodicalId":8234,"journal":{"name":"Annual review of chemical and biomolecular engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2021-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39071351","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 56
Introduction. 介绍。
IF 8.4 2区 工程技术 Q1 Chemical Engineering Pub Date : 2021-06-07 DOI: 10.1146/annurev-ch-12-033021-100001
Rachel A Segalman, Michael F Doherty
{"title":"Introduction.","authors":"Rachel A Segalman,&nbsp;Michael F Doherty","doi":"10.1146/annurev-ch-12-033021-100001","DOIUrl":"https://doi.org/10.1146/annurev-ch-12-033021-100001","url":null,"abstract":"","PeriodicalId":8234,"journal":{"name":"Annual review of chemical and biomolecular engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2021-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39071352","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Tough Double Network Hydrogel and Its Biomedical Applications. 强韧双网水凝胶及其生物医学应用。
IF 8.4 2区 工程技术 Q1 Chemical Engineering Pub Date : 2021-06-07 Epub Date: 2021-03-26 DOI: 10.1146/annurev-chembioeng-101220-080338
Takayuki Nonoyama, Jian Ping Gong

Soft and wet hydrogels have many similarities to biological tissues, though their mechanical fragility had been one of the biggest obstacles in biomedical applications. Studies and developments in double network (DN) hydrogels have elucidated how to create tough gels universally based on sacrificial bond principles and opened a path for biomedical application of hydrogels in regenerative medicine and artificial soft connective tissues, such as cartilage, tendon, and ligament, which endure high tension and compression. This review explores a universal toughening mechanism for and biomedical studies of DN hydrogels. Moreover, because the term sacrificial bonds has been mentioned often in studies of bone tissues, consisting of biomacromolecules and biominerals, recent studies of gel-biomineral composites to understand early-stage osteogenesis and to simulate bony sacrificial bonds are also summarized.

柔软和潮湿的水凝胶与生物组织有许多相似之处,尽管它们的机械脆弱性一直是生物医学应用的最大障碍之一。双网(DN)水凝胶的研究和发展阐明了如何基于牺牲键原理制造普遍具有韧性的凝胶,为水凝胶在再生医学和软骨、肌腱、韧带等承受高张力和压迫的人工软结缔组织的生物医学应用开辟了道路。本文综述了脱氧核糖核酸水凝胶的普遍增韧机理及其生物医学研究。此外,由于“牺牲键”一词在由生物大分子和生物矿物组成的骨组织的研究中经常被提及,本文也对近年来凝胶-生物矿物复合材料用于理解早期成骨和模拟骨牺牲键的研究进行了总结。
{"title":"Tough Double Network Hydrogel and Its Biomedical Applications.","authors":"Takayuki Nonoyama,&nbsp;Jian Ping Gong","doi":"10.1146/annurev-chembioeng-101220-080338","DOIUrl":"https://doi.org/10.1146/annurev-chembioeng-101220-080338","url":null,"abstract":"<p><p>Soft and wet hydrogels have many similarities to biological tissues, though their mechanical fragility had been one of the biggest obstacles in biomedical applications. Studies and developments in double network (DN) hydrogels have elucidated how to create tough gels universally based on sacrificial bond principles and opened a path for biomedical application of hydrogels in regenerative medicine and artificial soft connective tissues, such as cartilage, tendon, and ligament, which endure high tension and compression. This review explores a universal toughening mechanism for and biomedical studies of DN hydrogels. Moreover, because the term sacrificial bonds has been mentioned often in studies of bone tissues, consisting of biomacromolecules and biominerals, recent studies of gel-biomineral composites to understand early-stage osteogenesis and to simulate bony sacrificial bonds are also summarized.</p>","PeriodicalId":8234,"journal":{"name":"Annual review of chemical and biomolecular engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2021-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"25520081","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 43
RNA Engineering for Public Health: Innovations in RNA-Based Diagnostics and Therapeutics. 公共卫生的RNA工程:基于RNA的诊断和治疗的创新。
IF 8.4 2区 工程技术 Q1 Chemical Engineering Pub Date : 2021-06-07 DOI: 10.1146/annurev-chembioeng-101420-014055
Walter Thavarajah, Laura M Hertz, David Z Bushhouse, Chloé M Archuleta, Julius B Lucks

RNA is essential for cellular function: From sensing intra- and extracellular signals to controlling gene expression, RNA mediates a diverse and expansive list of molecular processes. A long-standing goal of synthetic biology has been to develop RNA engineering principles that can be used to harness and reprogram these RNA-mediated processes to engineer biological systems to solve pressing global challenges. Recent advances in the field of RNA engineering are bringing this to fruition, enabling the creation of RNA-based tools to combat some of the most urgent public health crises. Specifically, new diagnostics using engineered RNAs are able to detect both pathogens and chemicals while generating an easily detectable fluorescent signal as an indicator. New classes of vaccines and therapeutics are also using engineered RNAs to target a wide range of genetic and pathogenic diseases. Here, we discuss the recent breakthroughs in RNA engineering enabling these innovations and examine how advances in RNA design promise to accelerate the impact of engineered RNA systems.

RNA对细胞功能至关重要:从感知细胞内和细胞外信号到控制基因表达,RNA介导了多种多样的分子过程。合成生物学的一个长期目标是开发RNA工程原理,可用于利用和重新编程这些RNA介导的过程,以设计生物系统来解决紧迫的全球挑战。RNA工程领域的最新进展正在实现这一目标,使基于RNA的工具得以创建,以应对一些最紧迫的公共卫生危机。具体来说,使用工程化rna的新诊断方法能够检测病原体和化学物质,同时产生易于检测的荧光信号作为指示器。新型疫苗和治疗方法也在使用工程化rna来针对广泛的遗传和致病性疾病。在这里,我们讨论了使这些创新成为可能的RNA工程的最新突破,并研究了RNA设计的进步如何有望加速工程RNA系统的影响。
{"title":"RNA Engineering for Public Health: Innovations in RNA-Based Diagnostics and Therapeutics.","authors":"Walter Thavarajah,&nbsp;Laura M Hertz,&nbsp;David Z Bushhouse,&nbsp;Chloé M Archuleta,&nbsp;Julius B Lucks","doi":"10.1146/annurev-chembioeng-101420-014055","DOIUrl":"https://doi.org/10.1146/annurev-chembioeng-101420-014055","url":null,"abstract":"<p><p>RNA is essential for cellular function: From sensing intra- and extracellular signals to controlling gene expression, RNA mediates a diverse and expansive list of molecular processes. A long-standing goal of synthetic biology has been to develop RNA engineering principles that can be used to harness and reprogram these RNA-mediated processes to engineer biological systems to solve pressing global challenges. Recent advances in the field of RNA engineering are bringing this to fruition, enabling the creation of RNA-based tools to combat some of the most urgent public health crises. Specifically, new diagnostics using engineered RNAs are able to detect both pathogens and chemicals while generating an easily detectable fluorescent signal as an indicator. New classes of vaccines and therapeutics are also using engineered RNAs to target a wide range of genetic and pathogenic diseases. Here, we discuss the recent breakthroughs in RNA engineering enabling these innovations and examine how advances in RNA design promise to accelerate the impact of engineered RNA systems.</p>","PeriodicalId":8234,"journal":{"name":"Annual review of chemical and biomolecular engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2021-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9714562/pdf/nihms-1849307.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"9178826","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 6
Phagosome-Bacteria Interactions from the Bottom Up. 吞噬体与细菌自下而上的相互作用。
IF 8.4 2区 工程技术 Q1 Chemical Engineering Pub Date : 2021-06-07 Epub Date: 2021-03-29 DOI: 10.1146/annurev-chembioeng-090920-015024
Darshan M Sivaloganathan, Mark P Brynildsen

When attempting to propagate infections, bacterial pathogens encounter phagocytes that encase them in vacuoles called phagosomes. Within phagosomes, bacteria are bombarded with a plethora of stresses that often lead to their demise. However, pathogens have evolved numerous strategies to counter those host defenses and facilitate survival. Given the importance of phagosome-bacteria interactions to infection outcomes, they represent a collection of targets that are of interest for next-generation antibacterials. To facilitate such therapies, different approaches can be employed to increase understanding of phagosome-bacteria interactions, and these can be classified broadly as top down (starting from intact systems and breaking down the importance of different parts) or bottom up (developing a knowledge base on simplified systems and progressively increasing complexity). Here we review knowledge of phagosomal compositions and bacterial survival tactics useful for bottom-up approaches, which are particularly relevant for the application of reaction engineering to quantify and predict the time evolution of biochemical species in these death-dealing vacuoles. Further, we highlight how understanding in this area can be built up through the combination of immunology, microbiology, and engineering.

当试图传播感染时,细菌病原体遇到吞噬细胞,吞噬细胞将它们包裹在称为吞噬体的液泡中。在吞噬体内,细菌受到过多的压力轰击,往往导致它们死亡。然而,病原体已经进化出许多策略来对抗宿主的防御并促进生存。鉴于吞噬体-细菌相互作用对感染结果的重要性,它们代表了下一代抗菌药物感兴趣的靶标集合。为了促进这种治疗,可以采用不同的方法来增加对吞噬体-细菌相互作用的理解,这些方法可以大致分为自顶向下(从完整的系统开始,分解不同部分的重要性)或自底向上(在简化的系统上开发知识库,并逐步增加复杂性)。在这里,我们回顾了吞噬体组成和细菌生存策略的知识,这些知识对于自下而上的方法非常有用,特别是与反应工程的应用有关,可以量化和预测这些致命液泡中生化物种的时间进化。此外,我们强调如何通过免疫学、微生物学和工程学的结合来建立对这一领域的理解。
{"title":"Phagosome-Bacteria Interactions from the Bottom Up.","authors":"Darshan M Sivaloganathan,&nbsp;Mark P Brynildsen","doi":"10.1146/annurev-chembioeng-090920-015024","DOIUrl":"https://doi.org/10.1146/annurev-chembioeng-090920-015024","url":null,"abstract":"<p><p>When attempting to propagate infections, bacterial pathogens encounter phagocytes that encase them in vacuoles called phagosomes. Within phagosomes, bacteria are bombarded with a plethora of stresses that often lead to their demise. However, pathogens have evolved numerous strategies to counter those host defenses and facilitate survival. Given the importance of phagosome-bacteria interactions to infection outcomes, they represent a collection of targets that are of interest for next-generation antibacterials. To facilitate such therapies, different approaches can be employed to increase understanding of phagosome-bacteria interactions, and these can be classified broadly as top down (starting from intact systems and breaking down the importance of different parts) or bottom up (developing a knowledge base on simplified systems and progressively increasing complexity). Here we review knowledge of phagosomal compositions and bacterial survival tactics useful for bottom-up approaches, which are particularly relevant for the application of reaction engineering to quantify and predict the time evolution of biochemical species in these death-dealing vacuoles. Further, we highlight how understanding in this area can be built up through the combination of immunology, microbiology, and engineering.</p>","PeriodicalId":8234,"journal":{"name":"Annual review of chemical and biomolecular engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2021-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"25529077","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 9
Engineering Advances in Spray Drying for Pharmaceuticals. 药品喷雾干燥的工程进展。
IF 8.4 2区 工程技术 Q1 Chemical Engineering Pub Date : 2021-06-07 Epub Date: 2021-03-29 DOI: 10.1146/annurev-chembioeng-091720-034106
John M Baumann, Molly S Adam, Joel D Wood

Spray drying is a versatile technology that has been applied widely in the chemical, food, and, most recently, pharmaceutical industries. This review focuses on engineering advances and the most significant applications of spray drying for pharmaceuticals. An in-depth view of the process and its use is provided for amorphous solid dispersions, a major, growing drug-delivery approach. Enhanced understanding of the relationship of spray-drying process parameters to final product quality attributes has made robust product development possible to address a wide range of pharmaceutical problem statements. Formulation and process optimization have leveraged the knowledge gained as the technology has matured, enabling improved process development from early feasibility screening through commercial applications. Spray drying's use for approved small-molecule oral products is highlighted, as are emerging applications specific to delivery of biologics and non-oral delivery of dry powders. Based on the changing landscape of the industry, significant future opportunities exist for pharmaceutical spray drying.

喷雾干燥是一种多功能技术,已广泛应用于化学,食品,以及最近,制药工业。本文综述了喷雾干燥的工程进展和最重要的应用。深入的过程和它的使用提供了无定形固体分散体,一个主要的,日益增长的药物输送方法。对喷雾干燥工艺参数与最终产品质量属性的关系的增强理解,使稳健的产品开发成为可能,以解决广泛的制药问题陈述。随着技术的成熟,配方和工艺优化利用了所获得的知识,使从早期可行性筛选到商业应用的工艺开发得到了改进。强调了喷雾干燥用于批准的小分子口服产品,以及用于生物制剂输送和非口服干燥粉末输送的新兴应用。基于不断变化的行业格局,制药喷雾干燥存在重大的未来机会。
{"title":"Engineering Advances in Spray Drying for Pharmaceuticals.","authors":"John M Baumann,&nbsp;Molly S Adam,&nbsp;Joel D Wood","doi":"10.1146/annurev-chembioeng-091720-034106","DOIUrl":"https://doi.org/10.1146/annurev-chembioeng-091720-034106","url":null,"abstract":"<p><p>Spray drying is a versatile technology that has been applied widely in the chemical, food, and, most recently, pharmaceutical industries. This review focuses on engineering advances and the most significant applications of spray drying for pharmaceuticals. An in-depth view of the process and its use is provided for amorphous solid dispersions, a major, growing drug-delivery approach. Enhanced understanding of the relationship of spray-drying process parameters to final product quality attributes has made robust product development possible to address a wide range of pharmaceutical problem statements. Formulation and process optimization have leveraged the knowledge gained as the technology has matured, enabling improved process development from early feasibility screening through commercial applications. Spray drying's use for approved small-molecule oral products is highlighted, as are emerging applications specific to delivery of biologics and non-oral delivery of dry powders. Based on the changing landscape of the industry, significant future opportunities exist for pharmaceutical spray drying.</p>","PeriodicalId":8234,"journal":{"name":"Annual review of chemical and biomolecular engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2021-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"25529079","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 22
Dynamic Interconversion of Metal Active Site Ensembles in Zeolite Catalysis. 沸石催化中金属活性位系群的动态相互转化。
IF 8.4 2区 工程技术 Q1 Chemical Engineering Pub Date : 2021-06-07 Epub Date: 2021-04-07 DOI: 10.1146/annurev-chembioeng-092120-010920
Siddarth H Krishna, Casey B Jones, Rajamani Gounder

Catalysis science is founded on understanding the structure, number, and reactivity of active sites. Kinetic models that consider active sites to be static and noninteracting entities are routinely successful in describing the behavior of heterogeneous catalysts. Yet, active site ensembles often restructure in response to their external environment and even during steady-state catalytic turnover, sometimes requiring non-mean-field kinetic treatments to describe distance-dependent interactions among sites. Such behavior is being recognized more frequently in modern catalysis research, with the advent of experimental methods to quantify turnover rates with increasing precision, an expanding arsenal of operando characterization tools, and computational descriptions of atomic structure and motion at chemical potentials and timescales increasingly relevant to reaction conditions. This review focuses on dynamic changes to metal active site ensembles on zeolite supports, which are silica-based crystalline materials substituted with Al that generate binding sites for isolated and low-nuclearity metal site ensembles. Metal sites can become solvated and mobilized during reaction, facilitating interactions among sites that change their nuclearity and function. Such intersite communication can be regulated by the zeolite support, resulting in non-single-site and potentially non-mean-field kinetic behavior arising from mechanisms of catalytic action that combine elements of those canonically associated with homogeneous and heterogeneous catalysis.We discuss recent literature examples that document dynamic active site behavior in metal-zeolites and outline methodologies to identify and interpret such behavior. We conclude with our outlook on future research directions to develop this evolving branch of catalysis science and harness it for practical applications.

催化科学是建立在了解活性位点的结构、数量和反应性的基础上的。考虑活性位点为静态和非相互作用实体的动力学模型通常成功地描述了多相催化剂的行为。然而,活性位点集合体经常根据外部环境甚至在稳态催化周转过程中进行重组,有时需要非平均场动力学处理来描述位点之间依赖距离的相互作用。这种行为在现代催化研究中得到了更频繁的认识,随着实验方法的出现,以越来越精确的方式量化周转率,操作分子表征工具的扩充,原子结构和运动的计算描述在化学势和时间尺度上与反应条件越来越相关。本文综述了沸石载体上金属活性位点群的动态变化,沸石载体是硅基晶体材料,取代铝,产生分离的低核金属位点群的结合位点。金属位在反应过程中被溶剂化和动员,促进了位之间的相互作用,改变了它们的核和功能。这种位点间的交流可以通过沸石载体来调节,从而导致非单位点和潜在的非平均场动力学行为,这是由催化作用机制引起的,它结合了那些通常与均相和非均相催化相关的元素。我们讨论了最近的文献例子,这些文献记录了金属沸石中的动态活性位点行为,并概述了识别和解释这种行为的方法。最后,我们展望了未来的研究方向,以发展这一不断发展的催化科学分支并将其用于实际应用。
{"title":"Dynamic Interconversion of Metal Active Site Ensembles in Zeolite Catalysis.","authors":"Siddarth H Krishna,&nbsp;Casey B Jones,&nbsp;Rajamani Gounder","doi":"10.1146/annurev-chembioeng-092120-010920","DOIUrl":"https://doi.org/10.1146/annurev-chembioeng-092120-010920","url":null,"abstract":"<p><p>Catalysis science is founded on understanding the structure, number, and reactivity of active sites. Kinetic models that consider active sites to be static and noninteracting entities are routinely successful in describing the behavior of heterogeneous catalysts. Yet, active site ensembles often restructure in response to their external environment and even during steady-state catalytic turnover, sometimes requiring non-mean-field kinetic treatments to describe distance-dependent interactions among sites. Such behavior is being recognized more frequently in modern catalysis research, with the advent of experimental methods to quantify turnover rates with increasing precision, an expanding arsenal of operando characterization tools, and computational descriptions of atomic structure and motion at chemical potentials and timescales increasingly relevant to reaction conditions. This review focuses on dynamic changes to metal active site ensembles on zeolite supports, which are silica-based crystalline materials substituted with Al that generate binding sites for isolated and low-nuclearity metal site ensembles. Metal sites can become solvated and mobilized during reaction, facilitating interactions among sites that change their nuclearity and function. Such intersite communication can be regulated by the zeolite support, resulting in non-single-site and potentially non-mean-field kinetic behavior arising from mechanisms of catalytic action that combine elements of those canonically associated with homogeneous and heterogeneous catalysis.We discuss recent literature examples that document dynamic active site behavior in metal-zeolites and outline methodologies to identify and interpret such behavior. We conclude with our outlook on future research directions to develop this evolving branch of catalysis science and harness it for practical applications.</p>","PeriodicalId":8234,"journal":{"name":"Annual review of chemical and biomolecular engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2021-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"25567336","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 12
Polymer-Infiltrated Nanoparticle Films Using Capillarity-Based Techniques: Toward Multifunctional Coatings and Membranes. 基于毛细管技术的聚合物渗透纳米颗粒膜:迈向多功能涂层和膜。
IF 8.4 2区 工程技术 Q1 Chemical Engineering Pub Date : 2021-06-07 DOI: 10.1146/annurev-chembioeng-101220-093836
R Bharath Venkatesh, Neha Manohar, Yiwei Qiang, Haonan Wang, Hong Huy Tran, Baekmin Q Kim, Anastasia Neuman, Tian Ren, Zahra Fakhraai, Robert A Riggleman, Kathleen J Stebe, Kevin Turner, Daeyeon Lee

Polymer-infiltrated nanoparticle films (PINFs) are a new class of nanocomposites that offer synergistic properties and functionality derived from unusually high fractions of nanomaterials. Recently, two versatile techniques,capillary rise infiltration (CaRI) and solvent-driven infiltration of polymer (SIP), have been introduced that exploit capillary forces in films of densely packed nanoparticles. In CaRI, a highly loaded PINF is produced by thermally induced wicking of polymer melt into the nanoparticle packing pores. In SIP, exposure of a polymer-nanoparticle bilayer to solvent vapor atmosphere induces capillary condensation of solvent in the pores of nanoparticle packing, leading to infiltration of polymer into the solvent-filled pores. CaRI/SIP PINFs show superior properties compared with polymer nanocomposite films made using traditional methods, including superb mechanical properties, thermal stability, heat transfer, and optical properties. This review discusses fundamental aspects of the infiltration process and highlights potential applications in separations, structural coatings, and polymer upcycling-a process to convert polymer wastes into useful chemicals.

聚合物渗透纳米颗粒薄膜(pfs)是一类新型的纳米复合材料,它具有协同性能和功能,来源于不同寻常的高含量纳米材料。近年来,引入了毛细管上升渗透(CaRI)和溶剂驱动聚合物渗透(SIP)两种多用途技术,利用毛细管力在密集堆积的纳米颗粒薄膜中进行渗透。在CaRI中,高负载的pif是通过热诱导聚合物熔体进入纳米颗粒填充孔而产生的。在SIP中,聚合物-纳米颗粒双分子层暴露于溶剂蒸汽气氛中,导致纳米颗粒填料孔隙中的溶剂发生毛细缩聚,导致聚合物渗入溶剂填充的孔隙中。与传统方法制备的聚合物纳米复合薄膜相比,CaRI/SIP pfs具有优异的机械性能、热稳定性、传热性能和光学性能。本文讨论了渗透过程的基本方面,并强调了渗透过程在分离、结构涂层和聚合物升级回收(将聚合物废物转化为有用化学品的过程)方面的潜在应用。
{"title":"Polymer-Infiltrated Nanoparticle Films Using Capillarity-Based Techniques: Toward Multifunctional Coatings and Membranes.","authors":"R Bharath Venkatesh,&nbsp;Neha Manohar,&nbsp;Yiwei Qiang,&nbsp;Haonan Wang,&nbsp;Hong Huy Tran,&nbsp;Baekmin Q Kim,&nbsp;Anastasia Neuman,&nbsp;Tian Ren,&nbsp;Zahra Fakhraai,&nbsp;Robert A Riggleman,&nbsp;Kathleen J Stebe,&nbsp;Kevin Turner,&nbsp;Daeyeon Lee","doi":"10.1146/annurev-chembioeng-101220-093836","DOIUrl":"https://doi.org/10.1146/annurev-chembioeng-101220-093836","url":null,"abstract":"<p><p>Polymer-infiltrated nanoparticle films (PINFs) are a new class of nanocomposites that offer synergistic properties and functionality derived from unusually high fractions of nanomaterials. Recently, two versatile techniques,capillary rise infiltration (CaRI) and solvent-driven infiltration of polymer (SIP), have been introduced that exploit capillary forces in films of densely packed nanoparticles. In CaRI, a highly loaded PINF is produced by thermally induced wicking of polymer melt into the nanoparticle packing pores. In SIP, exposure of a polymer-nanoparticle bilayer to solvent vapor atmosphere induces capillary condensation of solvent in the pores of nanoparticle packing, leading to infiltration of polymer into the solvent-filled pores. CaRI/SIP PINFs show superior properties compared with polymer nanocomposite films made using traditional methods, including superb mechanical properties, thermal stability, heat transfer, and optical properties. This review discusses fundamental aspects of the infiltration process and highlights potential applications in separations, structural coatings, and polymer upcycling-a process to convert polymer wastes into useful chemicals.</p>","PeriodicalId":8234,"journal":{"name":"Annual review of chemical and biomolecular engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2021-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39071348","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 11
Nature-Inspired Chemical Engineering for Process Intensification. 过程强化的自然启发化学工程。
IF 8.4 2区 工程技术 Q1 Chemical Engineering Pub Date : 2021-06-07 Epub Date: 2021-03-31 DOI: 10.1146/annurev-chembioeng-060718-030249
Marc-Olivier Coppens

A nature-inspired solution (NIS) methodology is proposed as a systematic platform for innovation and to inform transformative technology required to address Grand Challenges, including sustainable development. Scalability, efficiency, and resilience are essential to nature, as they are to engineering processes. They are achieved through underpinning fundamental mechanisms, which are grouped as recurring themes in the NIS approach: hierarchical transport networks, force balancing, dynamic self-organization, and ecosystem properties. To leverage these universal mechanisms, and incorporate them effectively into engineering design, adaptations may be needed to accommodate the different contexts of nature and engineering applications. Nature-inspired chemical engineering takes advantage of the NIS methodology for process intensification, as demonstrated here in fluidization, catalysis, fuel cell engineering, and membrane separations, where much higher performance is achieved by rigorously employing concepts optimized in nature. The same approach lends itself to other applications, from biomedical engineering to information technology and architecture.

提出了一种自然启发的解决方案(NIS)方法,作为一个系统的创新平台,并为应对包括可持续发展在内的重大挑战所需的变革性技术提供信息。可伸缩性、效率和弹性对于自然是必不可少的,就像它们对于工程过程一样。它们是通过支撑基本机制实现的,这些机制在NIS方法中被归类为反复出现的主题:分层运输网络、力量平衡、动态自组织和生态系统属性。为了利用这些通用机制,并将它们有效地整合到工程设计中,可能需要调整以适应不同的自然环境和工程应用程序。受自然启发的化学工程利用NIS方法进行过程强化,如在流化,催化,燃料电池工程和膜分离中所展示的那样,通过严格采用自然优化的概念,可以实现更高的性能。同样的方法也适用于其他应用,从生物医学工程到信息技术和建筑。
{"title":"Nature-Inspired Chemical Engineering for Process Intensification.","authors":"Marc-Olivier Coppens","doi":"10.1146/annurev-chembioeng-060718-030249","DOIUrl":"https://doi.org/10.1146/annurev-chembioeng-060718-030249","url":null,"abstract":"<p><p>A nature-inspired solution (NIS) methodology is proposed as a systematic platform for innovation and to inform transformative technology required to address Grand Challenges, including sustainable development. Scalability, efficiency, and resilience are essential to nature, as they are to engineering processes. They are achieved through underpinning fundamental mechanisms, which are grouped as recurring themes in the NIS approach: hierarchical transport networks, force balancing, dynamic self-organization, and ecosystem properties. To leverage these universal mechanisms, and incorporate them effectively into engineering design, adaptations may be needed to accommodate the different contexts of nature and engineering applications. Nature-inspired chemical engineering takes advantage of the NIS methodology for process intensification, as demonstrated here in fluidization, catalysis, fuel cell engineering, and membrane separations, where much higher performance is achieved by rigorously employing concepts optimized in nature. The same approach lends itself to other applications, from biomedical engineering to information technology and architecture.</p>","PeriodicalId":8234,"journal":{"name":"Annual review of chemical and biomolecular engineering","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2021-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"25549121","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 12
期刊
Annual review of chemical and biomolecular engineering
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1