Accounts of materials research最新文献

{"title":"Construction of Reaction System and Regulation of Catalyst Active Sites for Sustainable Ammonia Production","authors":"Zhe Meng, Miao-Miao Shi and Jun-Min Yan*, ","doi":"10.1021/accountsmr.4c0010310.1021/accountsmr.4c00103","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00103https://doi.org/10.1021/accountsmr.4c00103","url":null,"abstract":"<p >Ammonia (NH<sub>3</sub>) is widely used for human life and considered a green energy carrier without CO<sub>2</sub> emissions; thus, green and sustainable NH<sub>3</sub> synthesis is of great importance. The traditional Haber-Bosch process requires harsh conditions with serious environmental implications. Therefore, numerous research is focused on the efficient synthesis of NH<sub>3</sub> from abundant N<sub>2</sub>/air and water under ambient conditions, utilizing renewable energy sources. Despite the fact that the electrocatalytic N<sub>2</sub> reduction reaction (eNRR) is an ideal method for NH<sub>3</sub> synthesis, the NH<sub>3</sub> yield and Faradaic efficiency (FE) are severally hampered by the inertness of N<sub>2</sub>, impeding its industrial application. Various strategies have been proposed to synthesize highly efficient heterogeneous catalysts for N<sub>2</sub> adsorption and dissociation to improve NH<sub>3</sub> yield and FE. Besides, benefiting from the nonthermal plasma N<sub>2</sub> oxidation reaction (pNOR) and electrocatalytic nitrate/nitrite reduction reaction (eNO<sub><i>x</i></sub>RR), the two-step approach overcomes the limitations of eNRR, attracting significant interest. This strategy facilitates N<sub>2</sub> splitting, which is a crucial step in the synthesis of NH<sub>3</sub>. Additionally, eNO<sub><i>x</i></sub>RR involves complex intermediates, making it essential to investigate catalysts with high selectivity of NH<sub>3</sub>. Overall, through the optimization of catalysts and reaction systems, NH<sub>3</sub> can be synthesized with high efficiency. The two-step strategy is the most realistic process for mass NH<sub>3</sub> production, but several challenges still need to be addressed, including improving the overall energy efficiency and scaling up the technology for industrial applications.</p><p >In this Account, we present an overview of our recent efforts in the construction of the reaction system and regulation of catalyst active sites for sustainable and efficient NH<sub>3</sub> synthesis. First, we introduce the design principles of the catalysts, which should possess abundant stable active sites and moderate adsorption strength. Subsequently, a range of strategies is proposed to enhance the NH<sub>3</sub> synthesis performance of Au, Bi, Co, Cu, and other catalysts, including coordination tuning, defect construction, elemental regulation, and structural design for direct eNRR and the two-step method of pNOR-eNO<sub><i>x</i></sub>RR at ambient conditions. Additionally, we explore the NH<sub>3</sub> synthesis process at a large scale by scaling up the electrode and reactor. Furthermore, the separation and collection routes of NH<sub>3</sub> from electrolytes are also investigated to meet the requirements of various applications. Finally, a brief outlook is provided to discuss the catalyst optimization method, remaining challenges, and future perspectives of expanding production. This Account will offer","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 12","pages":"1457–1471 1457–1471"},"PeriodicalIF":14.0,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143127703","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Construction of Reaction System and Regulation of Catalyst Active Sites for Sustainable Ammonia Production","authors":"Zhe Meng, Miao-Miao Shi, Jun-Min Yan","doi":"10.1021/accountsmr.4c00103","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00103","url":null,"abstract":"Ammonia (NH₃) is widely used for human life and considered a green energy carrier without CO₂ emissions; thus, green and sustainable NH₃ synthesis is of great importance. The traditional Haber-Bosch process requires harsh conditions with serious environmental implications. Therefore, numerous research is focused on the efficient synthesis of NH₃ from abundant N₂/air and water under ambient conditions, utilizing renewable energy sources. Despite the fact that the electrocatalytic N₂ reduction reaction (eNRR) is an ideal method for NH₃ synthesis, the NH₃ yield and Faradaic efficiency (FE) are severally hampered by the inertness of N₂, impeding its industrial application. Various strategies have been proposed to synthesize highly efficient heterogeneous catalysts for N₂ adsorption and dissociation to improve NH₃ yield and FE. Besides, benefiting from the nonthermal plasma N₂ oxidation reaction (pNOR) and electrocatalytic nitrate/nitrite reduction reaction (eNO_<i>x</i>RR), the two-step approach overcomes the limitations of eNRR, attracting significant interest. This strategy facilitates N₂ splitting, which is a crucial step in the synthesis of NH₃. Additionally, eNO_<i>x</i>RR involves complex intermediates, making it essential to investigate catalysts with high selectivity of NH₃. Overall, through the optimization of catalysts and reaction systems, NH₃ can be synthesized with high efficiency. The two-step strategy is the most realistic process for mass NH₃ production, but several challenges still need to be addressed, including improving the overall energy efficiency and scaling up the technology for industrial applications.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"63 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142519841","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Boosting Oxidative Stress with Hydroxyethyl Starch Smart Nanomedicines to Eliminate Cancer Stem Cells","authors":"Zitao Fan,&nbsp;Xing Wang,&nbsp;Xiangliang Yang and Zifu Li*,&nbsp;","doi":"10.1021/accountsmr.4c0024010.1021/accountsmr.4c00240","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00240https://doi.org/10.1021/accountsmr.4c00240","url":null,"abstract":"<p >The significance of cancer stem cells (CSCs), a rare population of cells in tumor tissues, in biology and the treatment of solid malignancies has been widely appreciated for more than two decades. Due to a peculiar self-renewal capability, even one single cancer stem cell can grow into a bulk tumor mass. For this reason, CSCs have long been blamed as the major culprit of tumor initiation, tumor progression, treatment resistance, metastasis, and recurrence. Therefore, it has been postulated that targeting CSCs could provide tremendous clinical benefits for patients with solid tumors. Accumulating studies corroborated that CSCs maintained a tight regulation of redox homeostasis and that the fate of CSCs was extremely sensitive to elevated oxidative stress. Accordingly, a plethora of therapeutic drugs that can generate reactive oxygen species (ROS) have been leveraged to target CSCs. Nonetheless, few drugs or formulations that are capable of elevating oxidative stress have achieved clinical success for eliminating CSCs thus far.</p><p >Hydroxyethyl starch (HES) has been widely utilized as a plasma volume expander in clinical settings for more than 50 years. Owing to its merits of excellent biocompatibility and biodegradability, good water solubility and manufacture practice, and abundant hydroxy groups for easy chemical modifications, HES has attracted great attention for tumor-targeted drug delivery. Specifically, HES has been leveraged as a nanoparticle stabilizer, as a nanocarrier to conjugate with chemotherapeutic drugs by stimuli-responsive linkers, and as a hydrophilic polymer to link with hydrophobic polymers to form self-assembled nanoparticles. In this Account, we summarize HES smart nanomedicines, developed in our group during the past five years, that could boost oxidative stress for CSC elimination. According to their effects on redox homeostasis, we categorize these nanomedicines into three classes. The first ones are nanomedicines that could generate excessive ROS, by means of mitochondria-targeted photodynamic therapy (Mito-PDT), cuproptosis, and ferroptosis. The second groups of nanomedicines own the capability to counteract endogenous reducing substances via inhibiting glutaminolysis and depleting glutathione (GSH). The third types of nanomedicines simultaneously amplify ROS generation and suppress antioxidant agents through combination strategies of Mito-PDT plus glutaminolysis inhibition, chemical dynamic therapy (CDT) plus GSH depletion, and CDT plus GSH depletion as well as inhibition. These rationally designed nanomedicines not only suppress CSCs <i>in vitro</i> but also eliminate CSCs in numerous tumor-bearing mice models <i>in vivo</i>, giving novel insights into anti-CSC therapy. As HES is widely used in the clinic, these HES smart nanomedicines hold significant potential for clinical translation.</p>","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 12","pages":"1558–1570 1558–1570"},"PeriodicalIF":14.0,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143127699","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"From Anisotropic Molecules and Particles to Small-Scale Actuators and Robots: An Account of Polymerized Liquid Crystals","authors":"Negar Rajabi, Matthew Gene Scarfo, Cole Martin Fredericks, Ramón Santiago Herrera Restrepo, Azin Adibi, Hamed Shahsavan","doi":"10.1021/accountsmr.4c00187","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00187","url":null,"abstract":"Untethered small-scale (milli-, micro-, and nano-) soft robots promise minimally invasive and targeted medical procedures in tiny, flooded, and confined environments like inside the human body. Despite such potentials, small-scale robots have not yet found their way to real-world applications. This can be mainly attributed to the fundamental and technical challenges in the fabrication, powering, navigation, imaging, and closed-loop control of robots at submillimiter scales. Pertinent to this Account, the selection of building block materials of small-scale robots also poses a challenge that is directly related to their fabrication and function.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"25 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142488784","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Boosting Oxidative Stress with Hydroxyethyl Starch Smart Nanomedicines to Eliminate Cancer Stem Cells","authors":"Zitao Fan, Xing Wang, Xiangliang Yang, Zifu Li","doi":"10.1021/accountsmr.4c00240","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00240","url":null,"abstract":"The significance of cancer stem cells (CSCs), a rare population of cells in tumor tissues, in biology and the treatment of solid malignancies has been widely appreciated for more than two decades. Due to a peculiar self-renewal capability, even one single cancer stem cell can grow into a bulk tumor mass. For this reason, CSCs have long been blamed as the major culprit of tumor initiation, tumor progression, treatment resistance, metastasis, and recurrence. Therefore, it has been postulated that targeting CSCs could provide tremendous clinical benefits for patients with solid tumors. Accumulating studies corroborated that CSCs maintained a tight regulation of redox homeostasis and that the fate of CSCs was extremely sensitive to elevated oxidative stress. Accordingly, a plethora of therapeutic drugs that can generate reactive oxygen species (ROS) have been leveraged to target CSCs. Nonetheless, few drugs or formulations that are capable of elevating oxidative stress have achieved clinical success for eliminating CSCs thus far.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"211 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142488783","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"From Anisotropic Molecules and Particles to Small-Scale Actuators and Robots: An Account of Polymerized Liquid Crystals","authors":"Negar Rajabi,&nbsp;Matthew Gene Scarfo,&nbsp;Cole Martin Fredericks,&nbsp;Ramón Santiago Herrera Restrepo,&nbsp;Azin Adibi and Hamed Shahsavan*,&nbsp;","doi":"10.1021/accountsmr.4c0018710.1021/accountsmr.4c00187","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00187https://doi.org/10.1021/accountsmr.4c00187","url":null,"abstract":"&lt;p &gt;Untethered small-scale (milli-, micro-, and nano-) soft robots promise minimally invasive and targeted medical procedures in tiny, flooded, and confined environments like inside the human body. Despite such potentials, small-scale robots have not yet found their way to real-world applications. This can be mainly attributed to the fundamental and technical challenges in the fabrication, powering, navigation, imaging, and closed-loop control of robots at submillimiter scales. Pertinent to this Account, the selection of building block materials of small-scale robots also poses a challenge that is directly related to their fabrication and function.&lt;/p&gt;&lt;p &gt;Early work in microrobotics focused on the mechanism of locomotion in fluids with low Reynolds number (&lt;i&gt;Re&lt;/i&gt; ≪ 1), which was mainly inspired by the motility of cells and microorganisms. Looking closely at the motile cells and microorganisms, one can find both order and anisotropy within their microstructure, driving out-of-equilibrium asymmetric deformations of their soft bodies and appendages like cilia and flagella, resulting in locomotion and function in environments with low &lt;i&gt;Re&lt;/i&gt; number. Microroboticists aim to mimic microorganisms’ locomotion and function in developing mobile small-scale robots. It is known that soft, ordered, and anisotropic microstructures of microorganisms are examples of liquid crystalline systems. With this in mind, we believe that liquid crystals are underutilized in the design of small-scale robots, even though they have remarkable similarities to biological materials and constructs.&lt;/p&gt;&lt;p &gt;In this Account, we have shed light on the role liquid crystals have played and can play in the design of small-scale robots. For this, we have first elaborated on the fundamentals of liquid crystals, which include a discussion of the various types of liquid crystals and their characteristics, their mesophase behavior, and their anisotropic properties. Then, we have discussed the applicability of anisotropic elastic networks of liquid crystals in the design of actuators which must satisfy all four programming pillars, including elasticity, alignment, responsiveness, and initial geometry. We have highlighted landmark reports where anisotropic elastic networks of liquid crystals, such as liquid crystal elastomers (LCEs), networks (LCNs), and hydrogels, are utilized as structural materials in the design of soft, small-scale actuators and robots. We point out the prevalence of the nematic phase and thermotropic liquid crystals utilized in these constructs over other mesophases and liquid crystal types as part of our discussion on the pros and cons of liquid crystals for microrobotics research. Finally, paths forward for the widespread applicability of liquid crystal microrobotics are envisaged. Specifically, the potential of soft robots constructed from elastic networks of chromonic and micellar lyotropic liquid crystals provides a substantial, yet daunting, opportunity f","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 12","pages":"1520–1531 1520–1531"},"PeriodicalIF":14.0,"publicationDate":"2024-10-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143127700","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Living Biomaterials: Fabrication Strategies and Biomedical Applications","authors":"Qi-Wen Chen, Xian-Zheng Zhang","doi":"10.1021/accountsmr.4c00258","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00258","url":null,"abstract":"Natural or bioengineered living organisms (including mammalian cells, bacteria, microalgaes, yeast, viruses, plant cells, and the multiple organism community) possess many intrinsic or artificial superiorities than the synthesized and inert biomaterials for application in many fields, especially biomedical applications. By leveraging the inherent or artificial therapeutic competences (e.g., disease chemotaxis, drugs production, intelligent delivery, immune activation and metabolic regulation), these living organisms have been developed as critical therapeutic formulations for biomedical applications to solve unmet medical needs. These living organisms are more intelligent, more easily available, more highly active, and more strongly curative than conventional inert formulations, such as inorganic nanocarriers, metal–organic chelating networks, polymeric nanovesicles and biomembrane biohybrids, etc. Nevertheless, nonspecific <i>in vivo</i> circulation, the diseased microenvironment-triggered inactivation, uncontrolled proliferation or colonization, unexpected side effects, and unsatisfactory therapeutic effect severely restricted their further research development and clinical approval. Living biomaterials, fabricated by integrating tailored functional materials with natural or bioengineered living organisms by chemical conjugation, physical assembly, and biological engineering strategies as well as advanced construction techniques, are rapidly developed to preserve or augment bioactivity and therapeutic properties of living organisms and even control their behaviors, decrease their biotoxicity, and impart them with new biofunctionalities, like stress resistance, bioactivity maintenance, safe trafficking, controllable proliferation and colonization, and evolved metabolism properties. These acquired capacities are especially beneficial to improve therapeutic potency and compliance, solve significant therapeutic restrictions, avoid biosafety questions, enhance therapeutic performances, and extend the boundaries of the fabricated living biomaterials on science research and practical biomedical applications. Additionally, the introduction of biocompatible and instructive functional materials, such as inorganic materials, synthetic polymers and polypeptides, functional proteins and enzymes, as well as biological component materials, can also promote the interaction of living biomaterials with the living body and provide feedback to further adapt the biofunctions of living organisms.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"13 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142488032","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Living Biomaterials: Fabrication Strategies and Biomedical Applications","authors":"Qi-Wen Chen,&nbsp; and ,&nbsp;Xian-Zheng Zhang*,&nbsp;","doi":"10.1021/accountsmr.4c0025810.1021/accountsmr.4c00258","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00258https://doi.org/10.1021/accountsmr.4c00258","url":null,"abstract":"&lt;p &gt;Natural or bioengineered living organisms (including mammalian cells, bacteria, microalgaes, yeast, viruses, plant cells, and the multiple organism community) possess many intrinsic or artificial superiorities than the synthesized and inert biomaterials for application in many fields, especially biomedical applications. By leveraging the inherent or artificial therapeutic competences (e.g., disease chemotaxis, drugs production, intelligent delivery, immune activation and metabolic regulation), these living organisms have been developed as critical therapeutic formulations for biomedical applications to solve unmet medical needs. These living organisms are more intelligent, more easily available, more highly active, and more strongly curative than conventional inert formulations, such as inorganic nanocarriers, metal–organic chelating networks, polymeric nanovesicles and biomembrane biohybrids, etc. Nevertheless, nonspecific &lt;i&gt;in vivo&lt;/i&gt; circulation, the diseased microenvironment-triggered inactivation, uncontrolled proliferation or colonization, unexpected side effects, and unsatisfactory therapeutic effect severely restricted their further research development and clinical approval. Living biomaterials, fabricated by integrating tailored functional materials with natural or bioengineered living organisms by chemical conjugation, physical assembly, and biological engineering strategies as well as advanced construction techniques, are rapidly developed to preserve or augment bioactivity and therapeutic properties of living organisms and even control their behaviors, decrease their biotoxicity, and impart them with new biofunctionalities, like stress resistance, bioactivity maintenance, safe trafficking, controllable proliferation and colonization, and evolved metabolism properties. These acquired capacities are especially beneficial to improve therapeutic potency and compliance, solve significant therapeutic restrictions, avoid biosafety questions, enhance therapeutic performances, and extend the boundaries of the fabricated living biomaterials on science research and practical biomedical applications. Additionally, the introduction of biocompatible and instructive functional materials, such as inorganic materials, synthetic polymers and polypeptides, functional proteins and enzymes, as well as biological component materials, can also promote the interaction of living biomaterials with the living body and provide feedback to further adapt the biofunctions of living organisms.&lt;/p&gt;&lt;p &gt;In this Account, we present a brief overview of recent advances of living biomaterials in their fabrication strategies and biomedical applications, embracing living organism species as well as living organism communities. We introduce the typical and practicable methods and techniques for fabrication of living biomaterials, mainly including chemical conjugation, physical assembly, biological editing, and metabolic engineering. On the basis of these fabrication st","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 11","pages":"1440–1452 1440–1452"},"PeriodicalIF":14.0,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691362","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Chemical Bonding Engineering: Insights into Physicochemical Performance Optimization for Energy-Storage/Conversion","authors":"Zhifang Zhou, Rui Wei, Xuefan Zhou, Yuan Liu, Dou Zhang, Yuan-Hua Lin","doi":"10.1021/accountsmr.4c00243","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00243","url":null,"abstract":"Chemical bonding is fundamental in determining the physicochemical properties of the materials. Establishing correlations between chemical bonding and these properties may help identify potential materials with unique advantages or guide the composition design for improving the performance of functional materials. However, there is a lack of literature addressing this issue. This Account examines how chemical bonding engineering affects the performance optimization of four widely used or investigated functional materials that are applied in energy-storage/conversion fields, including thermoelectrics, piezoelectrics, lithium-ion batteries (LIBs), and catalysts. The key issues of these materials and correlations between chemical bonding and properties are briefly summarized.","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"24 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142440666","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Chemical Bonding Engineering: Insights into Physicochemical Performance Optimization for Energy-Storage/Conversion","authors":"Zhifang Zhou,&nbsp;Rui Wei,&nbsp;Xuefan Zhou,&nbsp;Yuan Liu,&nbsp;Dou Zhang and Yuan-Hua Lin*,&nbsp;","doi":"10.1021/accountsmr.4c0024310.1021/accountsmr.4c00243","DOIUrl":"https://doi.org/10.1021/accountsmr.4c00243https://doi.org/10.1021/accountsmr.4c00243","url":null,"abstract":"&lt;p &gt;Chemical bonding is fundamental in determining the physicochemical properties of the materials. Establishing correlations between chemical bonding and these properties may help identify potential materials with unique advantages or guide the composition design for improving the performance of functional materials. However, there is a lack of literature addressing this issue. This Account examines how chemical bonding engineering affects the performance optimization of four widely used or investigated functional materials that are applied in energy-storage/conversion fields, including thermoelectrics, piezoelectrics, lithium-ion batteries (LIBs), and catalysts. The key issues of these materials and correlations between chemical bonding and properties are briefly summarized.&lt;/p&gt;&lt;p &gt;First, electron–phonon coupling hinders thermoelectric performance optimization, representing one of the main issues in the thermoelectric field that needs to be addressed. The role of chemical bonding engineering in electronic and phonon transport is discussed, highlighting how factors such as covalency, electronegativity differences, bond strength, and bond length affect carrier mobility and lattice thermal conductivity. We found that electronic and phonon transport properties can be tuned by modifying the chemical bonding of thermoelectric materials.&lt;/p&gt;&lt;p &gt;Second, the performance of perovskite piezoelectric materials is governed by their phase structure, which is closely associated with ABO&lt;sub&gt;3&lt;/sub&gt; lattice distortion. However, clarifying the correlations between perovskite distortion and chemical bonding has long been challenging. The effects of chemical bonding on perovskite distortion and ferroelectric/piezoelectric response are summarized, focusing on lead-free piezoelectric materials. The roles of ionic radii and electronic structures in the ionocovalent bonding between A-/B-site cations and oxygen anions, as well as the stability of perovskite structures, are discussed. These factors are proven to significantly affect the phase structure and piezoelectric response.&lt;/p&gt;&lt;p &gt;Third, during LIB operation, various chemical reactions occur within the electrodes and at the electrode/electrolyte interface, leading to the formation of new reversible or irreversible products. These structural and compositional changes signify a continuous evolution of the chemical bonds within the LIB system. Strategies to enhance the stability of high-capacity electrodes through the development of chemical cross-linker binders are summarized. Additionally, the impact of chemical bonds on the electrochemical stability and lithium-transport capabilities of solid-state electrolytes is also explored. Consequently, deliberately controlling chemical bonds is crucial for optimizing the overall electrochemical performance of LIBs, including parameters such as energy density, cycling lifespan, and fast-charging capabilities.&lt;/p&gt;&lt;p &gt;Fourthly, improving the catalytic activity of catalysts fo","PeriodicalId":72040,"journal":{"name":"Accounts of materials research","volume":"5 12","pages":"1571–1582 1571–1582"},"PeriodicalIF":14.0,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143127669","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}