Anthony U. Mu, Vibhu Vardhan Singh, Hyunyong Kim, Dong Ju Lee, Namseo Kim, Christian X. Ruff, Aaron Levy, Thomas A. Young, Francesco Paesani, Seth M. Cohen, Tod A. Pascal, Zheng Chen
{"title":"Structure–Activity Relationships in Ether-Functionalized Solid-State Metal–Organic Framework Electrolytes","authors":"Anthony U. Mu, Vibhu Vardhan Singh, Hyunyong Kim, Dong Ju Lee, Namseo Kim, Christian X. Ruff, Aaron Levy, Thomas A. Young, Francesco Paesani, Seth M. Cohen, Tod A. Pascal, Zheng Chen","doi":"10.1021/acs.chemmater.4c03384","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03384","url":null,"abstract":"The structure–property relationships of metal–organic framework (MOF)-based solid-state electrolytes are not well understood. Herein, a systematic investigation of 12 Zr(IV)-based UiO-66 MOFs with varying ether-chain functional groups was carried out to elucidate the critical microscopic interactions that facilitate improved solid-state electrolyte performance. Enhanced sampling molecular dynamics (MD) simulations were employed and revealed a three-tier ion hopping mechanism: linker–linker hopping, linker-counterion hopping, and counterion-counterion hopping. Detailed structural analysis of the MD trajectories revealed that the chemistry and morphology of the linker groups affect the relative stability and population distribution of the electrolyte components, such that crown-ether-based linker groups enhance the probability of extended, low-barrier ion percolation pathways. As a result, we were able to tune the ionic conductivities by rationally manipulating the counterion distributions, linker binding strengths, and the configurational entropy (multivariability of the linkers). The resulting performance of these MOF-based solid-state electrolytes was significantly enhanced, with a methoxy-functionalized framework (<b>UiO-66-L1</b><sub><b>100</b></sub>) achieving high ionic conductivities of 2.32 × 10<sup>–4</sup> S/cm and 2.07 × 10<sup>–3</sup> S/cm at 30 °C and 90 °C, respectively, an order of magnitude greater than other all-solid-state MOF electrolyte systems. The electrolyte stability was evaluated with LiIn|LPSCl|MOF:LiTFSI|LPSCl|LiIn symmetric cells, showing excellent Li plating/stripping processes for over 2 months.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"16 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798536","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chemistry of MaterialsPub Date : 2025-04-07DOI: 10.1021/acs.chemmater.4c0338410.1021/acs.chemmater.4c03384
Anthony U. Mu, Vibhu Vardhan Singh, Hyunyong Kim, Dong Ju Lee, Namseo Kim, Christian X. Ruff, Aaron Levy, Thomas A. Young, Francesco Paesani, Seth M. Cohen*, Tod A. Pascal* and Zheng Chen*,
{"title":"Structure–Activity Relationships in Ether-Functionalized Solid-State Metal–Organic Framework Electrolytes","authors":"Anthony U. Mu, Vibhu Vardhan Singh, Hyunyong Kim, Dong Ju Lee, Namseo Kim, Christian X. Ruff, Aaron Levy, Thomas A. Young, Francesco Paesani, Seth M. Cohen*, Tod A. Pascal* and Zheng Chen*, ","doi":"10.1021/acs.chemmater.4c0338410.1021/acs.chemmater.4c03384","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03384https://doi.org/10.1021/acs.chemmater.4c03384","url":null,"abstract":"<p >The structure–property relationships of metal–organic framework (MOF)-based solid-state electrolytes are not well understood. Herein, a systematic investigation of 12 Zr(IV)-based UiO-66 MOFs with varying ether-chain functional groups was carried out to elucidate the critical microscopic interactions that facilitate improved solid-state electrolyte performance. Enhanced sampling molecular dynamics (MD) simulations were employed and revealed a three-tier ion hopping mechanism: linker–linker hopping, linker-counterion hopping, and counterion-counterion hopping. Detailed structural analysis of the MD trajectories revealed that the chemistry and morphology of the linker groups affect the relative stability and population distribution of the electrolyte components, such that crown-ether-based linker groups enhance the probability of extended, low-barrier ion percolation pathways. As a result, we were able to tune the ionic conductivities by rationally manipulating the counterion distributions, linker binding strengths, and the configurational entropy (multivariability of the linkers). The resulting performance of these MOF-based solid-state electrolytes was significantly enhanced, with a methoxy-functionalized framework (<b>UiO-66-L1</b><sub><b>100</b></sub>) achieving high ionic conductivities of 2.32 × 10<sup>–4</sup> S/cm and 2.07 × 10<sup>–3</sup> S/cm at 30 °C and 90 °C, respectively, an order of magnitude greater than other all-solid-state MOF electrolyte systems. The electrolyte stability was evaluated with LiIn|LPSCl|MOF:LiTFSI|LPSCl|LiIn symmetric cells, showing excellent Li plating/stripping processes for over 2 months.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 8","pages":"2783–2794 2783–2794"},"PeriodicalIF":7.2,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853958","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"In Silico Exploration of Metabolite-Derived Soft Materials Using a Chemical Reaction Network","authors":"Shruti Iyer, Nicholas E. Jackson","doi":"10.1021/acs.chemmater.5c00163","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00163","url":null,"abstract":"Future soft materials and polymer chemistries will require innovative nonpetroleum sourcing pathways. While leveraging microbial metabolites derived from biological feedstocks possesses high potential in many avenues of chemical development, the applicability of this paradigm to the specifics of soft materials chemistry is unclear. Here, we construct a chemical reaction network based on databases of common microbial metabolites and the USPTO reaction set to examine what is possible in the chemical space of metabolite-derived chemistries of relevance to soft materials. We observe that the accessible chemical space of our chemical reaction network possesses strong microbe-specific chemical diversity and that this space saturates rapidly within three synthetic steps applied to the original microbial metabolites. Importantly, we show that the chemical space accessible from metabolite precursors possesses significant overlap with existing petrochemical building blocks, known and proposed synthetically feasible polymer monomers, and the chemical space of common organic semiconductors and redox active materials. The biases induced by the metabolite and reaction databases that parametrize our reaction network are analyzed as a function of chemical functional groups, and pathways toward broader sets of chemistries and reactions are outlined. This work introduces a computational framework for soft materials discovery with the potential to accelerate the identification of soft materials relevant to metabolic engineering targets and nonpetroleum sourcing pathways for existing soft materials.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"20 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776013","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Computational Ab Initio Approaches for Area-Selective Atomic Layer Deposition: Methods, Status, and Perspectives","authors":"Fabian Pieck, Ralf Tonner-Zech","doi":"10.1021/acs.chemmater.4c03477","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03477","url":null,"abstract":"Area-selective atomic layer deposition (AS-ALD) has emerged as a transformative technique in nanotechnology, enabling the precise deposition of materials on designated substrates while preventing unwanted growth on adjacent surfaces. This capability is critical for applications in microelectronics, catalysis, and energy technologies. Computational methods, particularly density functional theory (DFT), are indispensable for uncovering the mechanisms underlying AS-ALD, providing insights into surface interactions, selectivity mechanisms, and precursor design. This review introduces the theoretical background of computational techniques applied to AS-ALD and provides a detailed overview of their applications. Special emphasis is placed on the use of <i>ab initio</i> methods to explore surface chemistry, optimize precursor and inhibitor properties, and improve selectivity. A comprehensive overview of the literature is given with an analysis of research questions targeted, and methods used. By consolidating the state of knowledge and identifying future challenges, this work aims to guide researchers in further leveraging computational approaches to drive innovations in AS-ALD processes.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"89 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776012","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chemistry of MaterialsPub Date : 2025-04-04DOI: 10.1021/acs.chemmater.5c0016310.1021/acs.chemmater.5c00163
Shruti Iyer, and , Nicholas E. Jackson*,
{"title":"In Silico Exploration of Metabolite-Derived Soft Materials Using a Chemical Reaction Network","authors":"Shruti Iyer, and , Nicholas E. Jackson*, ","doi":"10.1021/acs.chemmater.5c0016310.1021/acs.chemmater.5c00163","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00163https://doi.org/10.1021/acs.chemmater.5c00163","url":null,"abstract":"<p >Future soft materials and polymer chemistries will require innovative nonpetroleum sourcing pathways. While leveraging microbial metabolites derived from biological feedstocks possesses high potential in many avenues of chemical development, the applicability of this paradigm to the specifics of soft materials chemistry is unclear. Here, we construct a chemical reaction network based on databases of common microbial metabolites and the USPTO reaction set to examine what is possible in the chemical space of metabolite-derived chemistries of relevance to soft materials. We observe that the accessible chemical space of our chemical reaction network possesses strong microbe-specific chemical diversity and that this space saturates rapidly within three synthetic steps applied to the original microbial metabolites. Importantly, we show that the chemical space accessible from metabolite precursors possesses significant overlap with existing petrochemical building blocks, known and proposed synthetically feasible polymer monomers, and the chemical space of common organic semiconductors and redox active materials. The biases induced by the metabolite and reaction databases that parametrize our reaction network are analyzed as a function of chemical functional groups, and pathways toward broader sets of chemistries and reactions are outlined. This work introduces a computational framework for soft materials discovery with the potential to accelerate the identification of soft materials relevant to metabolic engineering targets and nonpetroleum sourcing pathways for existing soft materials.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 8","pages":"2877–2888 2877–2888"},"PeriodicalIF":7.2,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143854006","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chemistry of MaterialsPub Date : 2025-04-04DOI: 10.1021/acs.chemmater.4c0327410.1021/acs.chemmater.4c03274
Elena Castagnotto*, Stefano Alberti, Marta Campolucci, Pietro Manfrinetti, Maurizio Ferretti and Federico Locardi*,
{"title":"Photocorrosion Stability of CdxZn1–xS Yellow-Orange Pigments","authors":"Elena Castagnotto*, Stefano Alberti, Marta Campolucci, Pietro Manfrinetti, Maurizio Ferretti and Federico Locardi*, ","doi":"10.1021/acs.chemmater.4c0327410.1021/acs.chemmater.4c03274","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03274https://doi.org/10.1021/acs.chemmater.4c03274","url":null,"abstract":"<p >Cadmium zinc sulfide pigments (Cd<sub><i>x</i></sub>Zn<sub>1–<i>x</i></sub>S) have been extensively used in art and industry for their bright colors. However, concerns exist over their long-term chemical stability. Due to their semiconductive properties under light exposure, these compounds may trigger photocatalytic processes that can lead to degradation issues in artworks. This study aims to replicate and compare the historical wet and dry synthesis of Cd<sub><i>x</i></sub>Zn<sub>1–<i>x</i></sub>S pigments and investigate their photocatalytic behavior, specifically their reactivity and ion leaching predispositions. Using adapted historical methods, we synthesized a series of Cd<sub><i>x</i></sub>Zn<sub>1–<i>x</i></sub>S pigments and fully characterized them using a range of analytical techniques. Their photocatalytic activity was evaluated against methylene blue dye under simulated sunlight, alongside a concomitant assessment of metal ion leaching. These experiments provide valuable insights into the historical pigments photocatalytic behavior, proposing key indicators of pigment reactivity in real artworks and demonstrating the origin of the inherent instability of historically synthesized pigments, particularly those made via wet methods. Under solar simulation, cubic nanosized pigments with 20% and 40% zinc content exhibit the highest degradation activity. This process is accompanied by the leaching of Cd<sup>2+</sup> and Zn<sup>2+</sup> ions, which may contribute to the formation of undesirable secondary products. The same pigments exhibited ion leaching even in the dark, although at significantly lower levels.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 8","pages":"2749–2761 2749–2761"},"PeriodicalIF":7.2,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143854143","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chemistry of MaterialsPub Date : 2025-04-04DOI: 10.1021/acs.chemmater.5c0028710.1021/acs.chemmater.5c00287
Henglong Li, Pengheng Li, Min Lin and Xing Zhu*,
{"title":"Effects of LaFeO3 Morphology on Oxygen Species and Chemical Looping Partial Oxidation of Methane","authors":"Henglong Li, Pengheng Li, Min Lin and Xing Zhu*, ","doi":"10.1021/acs.chemmater.5c0028710.1021/acs.chemmater.5c00287","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00287https://doi.org/10.1021/acs.chemmater.5c00287","url":null,"abstract":"<p >The design of oxygen carriers is essential for the chemical looping partial oxidation of methane (CL-POM) in syngas production. LaFeO<sub>3</sub> is a promising oxygen storage material, but the impact of its morphology on the reaction characteristics and mechanisms in CL-POM remains unclear. Herein, we synthesized and characterized LaFeO<sub>3</sub> samples with diverse morphologies (cube, porous microsphere, irregular nanoparticle, and polyhedron) to explore how morphology governs crystal plane exposure, oxygen vacancy formation, and oxygen migration. Results showed that cubic LaFeO<sub>3</sub> not only achieved outstanding oxygen storage capacity (4.18 mmol/g), 2.5 times that of the other three samples combined (1.64 mmol/g), but also demonstrated superior methane reactivity with good low-temperature activity (initial reaction temperature of 500 °C) and the highest methane conversion (78.26% at 750 °C). This impressive performance is due to the synergy between oxygen vacancies and the (110) crystal plane, which optimizes oxygen release and enhances methane adsorption and dissociation. DFT calculations further confirmed that the (110) plane has lower energy barriers for reaction processes than the (100) plane, and more oxygen vacancies enhance reactivity and oxygen migration. This work underscores the pivotal role of LaFeO<sub>3</sub> morphology in advancing the design of oxygen storage materials and a redox catalyst.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 8","pages":"2931–2942 2931–2942"},"PeriodicalIF":7.2,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143854147","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Effects of LaFeO3 Morphology on Oxygen Species and Chemical Looping Partial Oxidation of Methane","authors":"Henglong Li, Pengheng Li, Min Lin, Xing Zhu","doi":"10.1021/acs.chemmater.5c00287","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00287","url":null,"abstract":"The design of oxygen carriers is essential for the chemical looping partial oxidation of methane (CL-POM) in syngas production. LaFeO<sub>3</sub> is a promising oxygen storage material, but the impact of its morphology on the reaction characteristics and mechanisms in CL-POM remains unclear. Herein, we synthesized and characterized LaFeO<sub>3</sub> samples with diverse morphologies (cube, porous microsphere, irregular nanoparticle, and polyhedron) to explore how morphology governs crystal plane exposure, oxygen vacancy formation, and oxygen migration. Results showed that cubic LaFeO<sub>3</sub> not only achieved outstanding oxygen storage capacity (4.18 mmol/g), 2.5 times that of the other three samples combined (1.64 mmol/g), but also demonstrated superior methane reactivity with good low-temperature activity (initial reaction temperature of 500 °C) and the highest methane conversion (78.26% at 750 °C). This impressive performance is due to the synergy between oxygen vacancies and the (110) crystal plane, which optimizes oxygen release and enhances methane adsorption and dissociation. DFT calculations further confirmed that the (110) plane has lower energy barriers for reaction processes than the (100) plane, and more oxygen vacancies enhance reactivity and oxygen migration. This work underscores the pivotal role of LaFeO<sub>3</sub> morphology in advancing the design of oxygen storage materials and a redox catalyst.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"47 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776014","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Elena Castagnotto, Stefano Alberti, Marta Campolucci, Pietro Manfrinetti, Maurizio Ferretti, Federico Locardi
{"title":"Photocorrosion Stability of CdxZn1–xS Yellow-Orange Pigments","authors":"Elena Castagnotto, Stefano Alberti, Marta Campolucci, Pietro Manfrinetti, Maurizio Ferretti, Federico Locardi","doi":"10.1021/acs.chemmater.4c03274","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03274","url":null,"abstract":"Cadmium zinc sulfide pigments (Cd<sub><i>x</i></sub>Zn<sub>1–<i>x</i></sub>S) have been extensively used in art and industry for their bright colors. However, concerns exist over their long-term chemical stability. Due to their semiconductive properties under light exposure, these compounds may trigger photocatalytic processes that can lead to degradation issues in artworks. This study aims to replicate and compare the historical wet and dry synthesis of Cd<sub><i>x</i></sub>Zn<sub>1–<i>x</i></sub>S pigments and investigate their photocatalytic behavior, specifically their reactivity and ion leaching predispositions. Using adapted historical methods, we synthesized a series of Cd<sub><i>x</i></sub>Zn<sub>1–<i>x</i></sub>S pigments and fully characterized them using a range of analytical techniques. Their photocatalytic activity was evaluated against methylene blue dye under simulated sunlight, alongside a concomitant assessment of metal ion leaching. These experiments provide valuable insights into the historical pigments photocatalytic behavior, proposing key indicators of pigment reactivity in real artworks and demonstrating the origin of the inherent instability of historically synthesized pigments, particularly those made via wet methods. Under solar simulation, cubic nanosized pigments with 20% and 40% zinc content exhibit the highest degradation activity. This process is accompanied by the leaching of Cd<sup>2+</sup> and Zn<sup>2+</sup> ions, which may contribute to the formation of undesirable secondary products. The same pigments exhibited ion leaching even in the dark, although at significantly lower levels.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"18 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143782897","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xiang Zhang, Mingfei Xu, Zhi Kai Ng, Robert Vajtai, Edwin Hang Tong Teo, Yuji Zhao, Pulickel M. Ajayan
{"title":"Diamond: Recent Progress in Synthesis and Its Potential in Electronics","authors":"Xiang Zhang, Mingfei Xu, Zhi Kai Ng, Robert Vajtai, Edwin Hang Tong Teo, Yuji Zhao, Pulickel M. Ajayan","doi":"10.1021/acs.chemmater.5c00248","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00248","url":null,"abstract":"Diamond, with its extraordinary physical and electrical properties, has emerged as a transformative material for next-generation electronics. Its ultrawide bandgap, superior thermal conductivity, high carrier mobility, and excellent mechanical characteristics uniquely position it to address the limitations of traditional semiconductor materials. However, realizing the full potential of diamond in electronic applications requires overcoming significant challenges in its synthesis scalability, defect and dislocation control, and advanced device fabrication. In this Perspective, we discuss strategies and recent advancements in the synthesis of single-crystalline diamond in wafer scales as well as the reduction of defects and dislocations. The development of new diamond morphologies is also reviewed, underscoring their potential to modify properties and broaden application domains. Furthermore, we highlight the progress in engineering diamond-based electronic devices, particularly, field-effect transistors (FETs). Innovations in surface conductivity optimization and the realization of stable, normally off-device operation have enhanced the performance and reliability of diamond devices. Key areas for future research are proposed throughout, offering insights into the opportunities and challenges that remain in diamond synthesis and harnessing diamond’s full potential for next-generation electronic applications.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"16 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776020","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}