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Rational Design of Nanozymes for Engineered Cascade Catalytic Cancer Therapy
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-27 DOI: 10.1021/acs.chemrev.4c0088210.1021/acs.chemrev.4c00882
Xiuna Jia, Erkang Wang and Jin Wang*, 

Nanozymes have shown significant potential in cancer catalytic therapy by strategically catalyzing tumor-associated substances and metabolites into toxic reactive oxygen species (ROS) in situ, thereby inducing oxidative stress and promoting cancer cell death. However, within the complex tumor microenvironment (TME), the rational design of nanozymes and factors like activity, reaction substrates, and the TME itself significantly influence the efficiency of ROS generation. To address these limitations, recent research has focused on exploring the factors that affect activity and developing nanozyme-based cascade catalytic systems, which can trigger two or more cascade catalytic processes within tumors, thereby producing more therapeutic substances and achieving efficient and stable cancer therapy with minimal side effects. This area has shown remarkable progress. This Perspective provides a comprehensive overview of nanozymes, covering their classification and fundamentals. The regulation of nanozyme activity and efficient strategies of rational design are discussed in detail. Furthermore, representative paradigms for the successful construction of cascade catalytic systems for cancer treatment are summarized with a focus on revealing the underlying catalytic mechanisms. Finally, we address the current challenges and future prospects for the development of nanozyme-based cascade catalytic systems in biomedical applications.

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引用次数: 0
Beyond In Vivo, Pharmaceutical Molecule Production in Cell-Free Systems and the Use of Noncanonical Amino Acids Therein
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-22 DOI: 10.1021/acs.chemrev.4c0012610.1021/acs.chemrev.4c00126
Marco G. Casteleijn*, Ulrike Abendroth, Anne Zemella, Ruben Walter, Rashmi Rashmi, Rainer Haag and Stefan Kubick*, 

Throughout history, we have looked to nature to discover and copy pharmaceutical solutions to prevent and heal diseases. Due to the advances in metabolic engineering and the production of pharmaceutical proteins in different host cells, we have moved from mimicking nature to the delicate engineering of cells and proteins. We can now produce novel drug molecules, which are fusions of small chemical drugs and proteins. Currently we are at the brink of yet another step to venture beyond nature’s border with the use of unnatural amino acids and manufacturing without the use of living cells using cell-free systems. In this review, we summarize the progress and limitations of the last decades in the development of pharmaceutical protein development, production in cells, and cell-free systems. We also discuss possible future directions of the field.

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引用次数: 0
Beyond In Vivo, Pharmaceutical Molecule Production in Cell-Free Systems and the Use of Noncanonical Amino Acids Therein 在体内之外,无细胞系统中的药物分子生产和其中非规范氨基酸的使用
IF 62.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-22 DOI: 10.1021/acs.chemrev.4c00126
Marco G. Casteleijn, Ulrike Abendroth, Anne Zemella, Ruben Walter, Rashmi Rashmi, Rainer Haag, Stefan Kubick
Throughout history, we have looked to nature to discover and copy pharmaceutical solutions to prevent and heal diseases. Due to the advances in metabolic engineering and the production of pharmaceutical proteins in different host cells, we have moved from mimicking nature to the delicate engineering of cells and proteins. We can now produce novel drug molecules, which are fusions of small chemical drugs and proteins. Currently we are at the brink of yet another step to venture beyond nature’s border with the use of unnatural amino acids and manufacturing without the use of living cells using cell-free systems. In this review, we summarize the progress and limitations of the last decades in the development of pharmaceutical protein development, production in cells, and cell-free systems. We also discuss possible future directions of the field.
纵观历史,我们一直在向大自然寻求发现和复制药物解决方案,以预防和治疗疾病。由于代谢工程和在不同宿主细胞中生产药用蛋白的进展,我们已经从模仿自然转向细胞和蛋白质的精细工程。我们现在可以生产新的药物分子,它是小化学药物和蛋白质的融合物。目前,我们正处于冒险超越自然边界的另一步的边缘,使用非天然氨基酸和不使用活细胞的制造,使用无细胞系统。本文综述了近几十年来在药物蛋白的开发、细胞内生产和无细胞系统方面的进展和局限性。我们还讨论了该领域未来可能的发展方向。
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引用次数: 0
Protein-Based Degraders: From Chemical Biology Tools to Neo-Therapeutics
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-17 DOI: 10.1021/acs.chemrev.4c0059510.1021/acs.chemrev.4c00595
Lisha Ou, Mekedlawit T. Setegne, Jeandele Elliot, Fangfang Shen and Laura M. K. Dassama*, 

The nascent field of targeted protein degradation (TPD) could revolutionize biomedicine due to the ability of degrader molecules to selectively modulate disease-relevant proteins. A key limitation to the broad application of TPD is its dependence on small-molecule ligands to target proteins of interest. This leaves unstructured proteins or those lacking defined cavities for small-molecule binding out of the scope of many TPD technologies. The use of proteins, peptides, and nucleic acids (otherwise known as “biologics”) as the protein-targeting moieties in degraders addresses this limitation. In the following sections, we provide a comprehensive and critical review of studies that have used proteins and peptides to mediate the degradation and hence the functional control of otherwise challenging disease-relevant protein targets. We describe existing platforms for protein/peptide-based ligand identification and the drug delivery systems that might be exploited for the delivery of biologic-based degraders. Throughout the Review, we underscore the successes, challenges, and opportunities of using protein-based degraders as chemical biology tools to spur discoveries, elucidate mechanisms, and act as a new therapeutic modality.

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引用次数: 0
Protein-Based Degraders: From Chemical Biology Tools to Neo-Therapeutics 基于蛋白质的降解剂:从化学生物学工具到新疗法
IF 62.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-17 DOI: 10.1021/acs.chemrev.4c00595
Lisha Ou, Mekedlawit T. Setegne, Jeandele Elliot, Fangfang Shen, Laura M. K. Dassama
The nascent field of targeted protein degradation (TPD) could revolutionize biomedicine due to the ability of degrader molecules to selectively modulate disease-relevant proteins. A key limitation to the broad application of TPD is its dependence on small-molecule ligands to target proteins of interest. This leaves unstructured proteins or those lacking defined cavities for small-molecule binding out of the scope of many TPD technologies. The use of proteins, peptides, and nucleic acids (otherwise known as “biologics”) as the protein-targeting moieties in degraders addresses this limitation. In the following sections, we provide a comprehensive and critical review of studies that have used proteins and peptides to mediate the degradation and hence the functional control of otherwise challenging disease-relevant protein targets. We describe existing platforms for protein/peptide-based ligand identification and the drug delivery systems that might be exploited for the delivery of biologic-based degraders. Throughout the Review, we underscore the successes, challenges, and opportunities of using protein-based degraders as chemical biology tools to spur discoveries, elucidate mechanisms, and act as a new therapeutic modality.
由于降解分子有选择性地调节疾病相关蛋白的能力,靶向蛋白降解(TPD)这一新兴领域可能会给生物医学带来革命性的变化。TPD广泛应用的一个关键限制是它依赖于小分子配体来靶向感兴趣的蛋白质。这使得非结构化蛋白质或那些缺乏用于小分子结合的明确空腔的蛋白质超出了许多TPD技术的范围。使用蛋白质、多肽和核酸(也称为“生物制剂”)作为降解物中的蛋白质靶向部分解决了这一限制。在接下来的章节中,我们对使用蛋白质和肽介导降解的研究进行了全面和批判性的回顾,从而对其他具有挑战性的疾病相关蛋白质靶点进行了功能控制。我们描述了现有的基于蛋白质/肽的配体识别平台和可能用于递送生物基降解物的药物递送系统。在整个综述中,我们强调了使用基于蛋白质的降解物作为化学生物学工具的成功、挑战和机遇,以促进发现,阐明机制,并作为一种新的治疗方式。
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引用次数: 0
Hydrolysis, Ligand Exchange, and Redox Properties of Vanadium Compounds: Implications of Solution Transformation on Biological, Therapeutic, and Environmental Applications
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-16 DOI: 10.1021/acs.chemrev.4c0047510.1021/acs.chemrev.4c00475
Rupam Dinda*, Eugenio Garribba*, Daniele Sanna, Debbie C. Crans* and João Costa Pessoa*, 

Vanadium is a transition metal with important industrial, technological, biological, and biomedical applications widespread in the environment and in living beings. The different reactions that vanadium compounds (VCs) undergo in the presence of proteins, nucleic acids, lipids and metabolites under mild physiological conditions are reviewed. In the environment vanadium is present naturally or through anthropogenic sources, the latter having an environmental impact caused by the dispersion of VCs in the atmosphere and aquifers. Vanadium has a versatile chemistry with interconvertible oxidation states, variable coordination number and geometry, and ability to form polyoxidovanadates with various nuclearity and structures. If a VC is added to a water-containing environment it can undergo hydrolysis, ligand-exchange, redox, and other types of changes, determined by the conditions and speciation chemistry of vanadium. Importantly, the solution is likely to differ from the VC introduced into the system and varies with concentration. Here, vanadium redox, hydrolytic and ligand-exchange chemical reactions, the influence of pH, concentration, salt, specific solutes, biomolecules, and VCs on the speciation are described. One of our goals with this work is highlight the need for assessment of the VC speciation, so that beneficial or toxic species might be identified and mechanisms of action be elucidated.

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引用次数: 0
Hydrolysis, Ligand Exchange, and Redox Properties of Vanadium Compounds: Implications of Solution Transformation on Biological, Therapeutic, and Environmental Applications 钒化合物的水解、配体交换和氧化还原性质:溶液转化在生物、治疗和环境应用中的意义
IF 62.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-16 DOI: 10.1021/acs.chemrev.4c00475
Rupam Dinda, Eugenio Garribba, Daniele Sanna, Debbie C. Crans, João Costa Pessoa
Vanadium is a transition metal with important industrial, technological, biological, and biomedical applications widespread in the environment and in living beings. The different reactions that vanadium compounds (VCs) undergo in the presence of proteins, nucleic acids, lipids and metabolites under mild physiological conditions are reviewed. In the environment vanadium is present naturally or through anthropogenic sources, the latter having an environmental impact caused by the dispersion of VCs in the atmosphere and aquifers. Vanadium has a versatile chemistry with interconvertible oxidation states, variable coordination number and geometry, and ability to form polyoxidovanadates with various nuclearity and structures. If a VC is added to a water-containing environment it can undergo hydrolysis, ligand-exchange, redox, and other types of changes, determined by the conditions and speciation chemistry of vanadium. Importantly, the solution is likely to differ from the VC introduced into the system and varies with concentration. Here, vanadium redox, hydrolytic and ligand-exchange chemical reactions, the influence of pH, concentration, salt, specific solutes, biomolecules, and VCs on the speciation are described. One of our goals with this work is highlight the need for assessment of the VC speciation, so that beneficial or toxic species might be identified and mechanisms of action be elucidated.
钒是一种具有重要工业、技术、生物和生物医学应用的过渡金属,广泛存在于环境和生物体内。综述了钒化合物在蛋白质、核酸、脂质和代谢物存在下在温和生理条件下发生的不同反应。在环境中,钒是自然存在的或通过人为来源存在的,后者由于vc在大气和含水层中的分散而对环境产生影响。钒具有多种化学性质,氧化态可以相互转换,配位数和几何形状可以改变,并且能够形成具有不同核和结构的多氧化钒酸盐。如果VC被添加到含水的环境中,它可以发生水解、配体交换、氧化还原和其他类型的变化,这取决于钒的条件和形态化学。重要的是,溶液可能与引入系统的VC不同,并随浓度而变化。本文描述了钒的氧化还原、水解和配体交换化学反应,以及pH、浓度、盐、特定溶质、生物分子和vc对物种形成的影响。我们这项工作的目标之一是强调评估VC物种形成的必要性,以便确定有益或有毒的物种,并阐明其作用机制。
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引用次数: 0
The Impact of Electric Fields on Processes at Electrode Interfaces
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-16 DOI: 10.1021/acs.chemrev.4c0048710.1021/acs.chemrev.4c00487
Zhuoran Long, Jinhui Meng, Lydia R. Weddle, Pablo E. Videla, Jan Paul Menzel, Delmar G. A. Cabral, Jinchan Liu, Tianyin Qiu, Joseph M. Palasz, Dhritiman Bhattacharyya, Clifford P. Kubiak*, Victor S. Batista* and Tianquan Lian*, 

The application of external electric fields to influence chemical reactions at electrode interfaces has attracted considerable interest in recent years. However, the design of electric fields to achieve highly efficient and selective catalytic systems, akin to the optimized fields found at enzyme active sites, remains a significant challenge. Consequently, there has been substantial effort in probing and understanding the interfacial electric fields at electrode/electrolyte interfaces and their effect on adsorbates. In this review, we examine recent advances in experimental, computational, and theoretical studies of the interfacial electric field, the origin of the vibrational Stark effect of adsorbates on electrode surfaces, and the effects of electric fields on reactions at electrode/electrolyte interfaces. We also discuss recent advances in control of charge transfer and chemical reactions using magnetic fields. Finally, we outline perspectives on key areas for future studies.

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引用次数: 0
Interfacial Catalysis at Atomic Level
IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-16 DOI: 10.1021/acs.chemrev.4c0061810.1021/acs.chemrev.4c00618
Mi Peng, Chengyu Li, Zhaohua Wang, Maolin Wang, Qingxin Zhang, Bingjun Xu*, Mufan Li* and Ding Ma*, 

Heterogeneous catalysts are pivotal to the chemical and energy industries, which are central to a multitude of industrial processes. Large-scale industrial catalytic processes rely on special structures at the nano- or atomic level, where reactions proceed on the so-called active sites of heterogeneous catalysts. The complexity of these catalysts and active sites often lies in the interfacial regions where different components in the catalysts come into contact. Recent advances in synthetic methods, characterization technologies, and reaction kinetics studies have provided atomic-scale insights into these critical interfaces. Achieving atomic precision in interfacial engineering allows for the manipulation of electronic profiles, adsorption patterns, and surface motifs, deepening our understanding of reaction mechanisms at the atomic or molecular level. This mechanistic understanding is indispensable not only for fundamental scientific inquiry but also for the design of the next generation of highly efficient industrial catalysts. This review examines the latest developments in atomic-scale interfacial engineering, covering fundamental concepts, catalyst design, mechanistic insights, and characterization techniques, and shares our perspective on the future trajectory of this dynamic research field.

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引用次数: 0
The Impact of Electric Fields on Processes at Electrode Interfaces 电场对电极界面过程的影响
IF 62.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-16 DOI: 10.1021/acs.chemrev.4c00487
Zhuoran Long, Jinhui Meng, Lydia R. Weddle, Pablo E. Videla, Jan Paul Menzel, Delmar G. A. Cabral, Jinchan Liu, Tianyin Qiu, Joseph M. Palasz, Dhritiman Bhattacharyya, Clifford P. Kubiak, Victor S. Batista, Tianquan Lian
The application of external electric fields to influence chemical reactions at electrode interfaces has attracted considerable interest in recent years. However, the design of electric fields to achieve highly efficient and selective catalytic systems, akin to the optimized fields found at enzyme active sites, remains a significant challenge. Consequently, there has been substantial effort in probing and understanding the interfacial electric fields at electrode/electrolyte interfaces and their effect on adsorbates. In this review, we examine recent advances in experimental, computational, and theoretical studies of the interfacial electric field, the origin of the vibrational Stark effect of adsorbates on electrode surfaces, and the effects of electric fields on reactions at electrode/electrolyte interfaces. We also discuss recent advances in control of charge transfer and chemical reactions using magnetic fields. Finally, we outline perspectives on key areas for future studies.
近年来,应用外部电场来影响电极界面上的化学反应引起了人们的极大兴趣。然而,如何设计电场以实现高效和选择性催化系统(类似于酶活性位点的优化电场),仍然是一项重大挑战。因此,人们在探测和了解电极/电解质界面电场及其对吸附剂的影响方面付出了巨大努力。在本综述中,我们将探讨界面电场的实验、计算和理论研究的最新进展,电极表面吸附剂振动斯塔克效应的起源,以及电场对电极/电解质界面反应的影响。我们还讨论了利用磁场控制电荷转移和化学反应的最新进展。最后,我们对未来研究的关键领域进行了展望。
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引用次数: 0
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