Inorganic Chemistry Frontiers最新文献

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Enhancing upconversion luminescence via intermediate state in double perovskite phosphor: three-mode optical thermometry with python-assisted validation 通过双过氧化物荧光粉中的中间状态增强上转换发光:利用 python-assisted 验证的三模式光学测温仪
IF 7 1区 化学
Inorganic Chemistry Frontiers Pub Date : 2025-04-15 DOI: 10.1039/d5qi00572h
Ruitong Song, Sen Yan, Shihao Duan, Xin Yang, Esmond A. Balfour, Hao Fu
{"title":"Enhancing upconversion luminescence via intermediate state in double perovskite phosphor: three-mode optical thermometry with python-assisted validation","authors":"Ruitong Song, Sen Yan, Shihao Duan, Xin Yang, Esmond A. Balfour, Hao Fu","doi":"10.1039/d5qi00572h","DOIUrl":"https://doi.org/10.1039/d5qi00572h","url":null,"abstract":"High luminescence intensity, multiple modes, and high sensitivity are critical to achieving high measurement accuracy for optical thermometry in microelectronic devices and biological systems. The double perovskite phosphor, Ca2Sc0.63Mg0.07SbO6:Yb3+,Er3+, proves to be promising in overcoming these challenges. A simple high-temperature solid-phase method was used to prepare this sample which was found to exhibit red anti-Stokes luminescence under 980 nm excitation. Heterovalent substitution of Mg2+ for Sc3+ leads to lattice shrinkage and oxygen vacancy content enhancement. The induced generation of the intermediate state by the oxygen vacancy is significantly increased. This consequently enhances the upconversion luminescence intensity. The Ca2Sc0.63Mg0.07SbO6:Yb3+,Er3+ phosphor is capable of three-mode optical thermometry by thermally coupled energy states (TCES), non-thermally coupled energy states (NTCES), and CIE chromaticity shift. The NTCES-based mode has a notable relative sensitivity of Sr-max = 4.8% K-1 and superior signal resolution δT = 0.016 K. Furthermore, the NTCES-based model was tested for practical applications, and the difference between the predicted theoretical temperature and the actual test temperature was kept within 6 K after about 100,000 evaluations via Python assistance.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"74 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832238","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mechanism behind oxidase activity of cellulose-active AA10 lytic polysaccharide monooxygenases 纤维素活性AA10水解多糖单加氧酶氧化酶活性背后的机制
IF 7 1区 化学
Inorganic Chemistry Frontiers Pub Date : 2025-04-15 DOI: 10.1039/d5qi00796h
Erna Katharina Wieduwilt, Marlisa Muriel Hagemann, Ulf Ryde, Erik Donovan Hedegård
{"title":"Mechanism behind oxidase activity of cellulose-active AA10 lytic polysaccharide monooxygenases","authors":"Erna Katharina Wieduwilt, Marlisa Muriel Hagemann, Ulf Ryde, Erik Donovan Hedegård","doi":"10.1039/d5qi00796h","DOIUrl":"https://doi.org/10.1039/d5qi00796h","url":null,"abstract":"Lytic polysaccharide monooxygenases (LPMOs) are copper enzymes that boost the degradation of different polysaccharides and play important roles in the sustainable production of biofuels, in human and plant pathogens, and potentially also in plastic degradation. Their activity depends on a co-substrate, where recent results show that hydrogen peroxide is the preferred co-substrate. Under typical experimental conditions, no hydrogen peroxide is added and it is instead produced <em>in situ</em> by LPMOs themselves, which could be the rate-limiting step. Previous theoretical investigations of the oxidase reaction have been highly inhomogeneous, and focused on different aspects of LPMO reactivity. In this paper, we systematically investigate how LPMOs generate hydrogen peroxide using accurate quantum mechanics/molecular mechanics (QM/MM) hybrid methods with extended QM regions. We find that the reaction of the reduced LPMO active site with O<small><sub>2</sub></small> yields a superoxide coordinated to Cu(II), from which [Cu(II)-OOH<small><sup>-</sup></small>]<small><sup>+</sup></small> can be formed via a proton-coupled electron transfer, using a second-coordination-sphere histidine as proton donor. Either OOH<small><sup>–</sup></small> dissociates from this species (while abstracting a proton from a water molecule) or [Cu(II)−OOH<small><sup>–</sup></small> ]<small><sup>+</sup></small> reacts in a second protonation from the second-sphere histidine, yielding [Cu(II)−H<small><sub>2</sub></small>O<small><sub>2</sub></small> ]<small><sup>2+</sup></small>, followed by dissociation of H<small><sub>2</sub></small>O<small><sub>2</sub></small>. Energetically, all three oxygen species can dissociate into solution, but the dissociation of H<small><sub>2</sub></small>O<small><sub>2</sub></small> from the Cu(II) active-site is the most favorable while dissociation of O<small><sub>2</sub></small><small><sup>.-</sup></small> is least favorable.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"72 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832235","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Insights for controlling plutonium behavior in hydrochloric acid solutions 控制盐酸溶液中钚行为的见解
IF 7 1区 化学
Inorganic Chemistry Frontiers Pub Date : 2025-04-14 DOI: 10.1039/d5qi00409h
Yufei Wang, Natalie T. Rice, Julia G. Knapp, Sara L. Adelman, Kelly E. Aldrich, Brian T. Arko, Manuel L. Besmer, J. Connor Gilhula, Christopher J. Godt, Jan Klouda, Stosh A. Kozimor, Brian N. Long, Molly M. MacInnes, Travis Marshall-Roth, Alexandra L. Nagelski, Ida D. Piedmonte
{"title":"Insights for controlling plutonium behavior in hydrochloric acid solutions","authors":"Yufei Wang, Natalie T. Rice, Julia G. Knapp, Sara L. Adelman, Kelly E. Aldrich, Brian T. Arko, Manuel L. Besmer, J. Connor Gilhula, Christopher J. Godt, Jan Klouda, Stosh A. Kozimor, Brian N. Long, Molly M. MacInnes, Travis Marshall-Roth, Alexandra L. Nagelski, Ida D. Piedmonte","doi":"10.1039/d5qi00409h","DOIUrl":"https://doi.org/10.1039/d5qi00409h","url":null,"abstract":"Advancing understanding of aqueous chemistry for plutonium is important because it impacts energy production, environmental management, and national security. Unfortunately, plutonium's aqueous chemistry remains poorly characterized. We addressed this problem by characterizing Pu(<small>IV</small>) redox and coordination chemistry in aqueous solutions as a function of hydrochloric acid concentration using X-ray absorption spectroscopy, ultraviolet-visible near-infrared spectroscopy, and electrochemistry. The impact of Pu–Cl <em>vs.</em> Pu–O<small><sub>H<small><sub>2</sub></small>O</sub></small> bonding was correlated with the stability of different plutonium oxidation states. We discovered that anionic Cl<small><sup>1−</sup></small> ligands stabilized electron-deficient Pu(<small>IV</small>) over Pu(<small>III</small>) and neutral H<small><sub>2</sub></small>O ligands stabilized Pu(<small>III</small>) over Pu(<small>IV</small>). These findings offer a way to control plutonium electron transfer chemistry and imply that selective stabilization of Pu(<small>IV</small>) or Pu(<small>III</small>) may be achieved through tuning the electron donating ability of the ligand. Overall, this work advances predictive capabilities for aqueous plutonium chemistry, particularly within nuclear application spaces.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"17 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827492","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synergistic Coordination in 89Zr-DFO (Deferoxamine) Complexes: Computational and Experimental Insights into Auxiliary Ligands 89Zr-DFO(脱氧胺)配合物中的协同配位:计算和实验对辅助配体的启示
IF 7 1区 化学
Inorganic Chemistry Frontiers Pub Date : 2025-04-14 DOI: 10.1039/d5qi00879d
Jiarui Li, Chenghe Ding, Yang Gao, Lili Wen, Pingping Zhao, Lu Zhou, Rui Luo, Mingsong Shi, Georg Schreckenbach, Xiaoan Li, Zhiming Wang
{"title":"Synergistic Coordination in 89Zr-DFO (Deferoxamine) Complexes: Computational and Experimental Insights into Auxiliary Ligands","authors":"Jiarui Li, Chenghe Ding, Yang Gao, Lili Wen, Pingping Zhao, Lu Zhou, Rui Luo, Mingsong Shi, Georg Schreckenbach, Xiaoan Li, Zhiming Wang","doi":"10.1039/d5qi00879d","DOIUrl":"https://doi.org/10.1039/d5qi00879d","url":null,"abstract":"This study combines computational and experimental methods to investigate how auxiliary ligands enhance thermodynamic stability in hexacoordinate <small><sup>89</sup></small>Zr-DFO (Deferoxamine) complexes. Strong electrostatic interactions favour HPO<small><sub>4</sub></small><small><sup>2-</sup></small> over H<small><sub>2</sub></small>O, Cl<small><sup>-</sup></small>, CO<small><sub>3</sub></small><small><sup>2-</sup></small> and C<small><sub>2</sub></small>O<small><sub>4</sub></small><small><sup>2-</sup></small>, indicating superior stability for advanced medical diagnostics and treatment applications.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"26 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832241","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Efficient photooxidation of C(sp3)-H bonds on visible-light-responsive W-doped TiO2 nanocrystals promoted by photochromic effect 光致变色效应促进可见光响应w掺杂TiO2纳米晶体上C(sp3)-H键的高效光氧化
IF 7 1区 化学
Inorganic Chemistry Frontiers Pub Date : 2025-04-11 DOI: 10.1039/d5qi00131e
Zhen Zhang, Yun Zhang, Chaowei Han, Mei Yan, Guanfeng Ji, Wenshou Wang
{"title":"Efficient photooxidation of C(sp3)-H bonds on visible-light-responsive W-doped TiO2 nanocrystals promoted by photochromic effect","authors":"Zhen Zhang, Yun Zhang, Chaowei Han, Mei Yan, Guanfeng Ji, Wenshou Wang","doi":"10.1039/d5qi00131e","DOIUrl":"https://doi.org/10.1039/d5qi00131e","url":null,"abstract":"Photocatalytic oxidation of C(sp3)-H bonds using semiconducting catalysts is crucial for value-added chemical production under milder conditions. However, semiconductor-based photocatalysts often suffer from limited active sites and low photoredox activity. Herein, we report W-doped TiO2 nanocrystals that exhibit a photochromic behavior for photocatalytic oxidation of C(sp3)-H bonds with high efficiencies. The photochromic effect induced W5+-Ovs-Ti3+ (oxygen vacancies short as Ovs) active sites in TiO2 nanocrystals act as electron trapping centers to capture and store photogenerated electrons, promoting the photogenerated holes to active C(sp3)-H bonds. Moreover, the Ovs and stored photogenerated electrons on the active sites significantly enhance the adsorption and activation of O2 to O2•-. Owing to the unique photochromic effect, the W-doped TiO2 nanocrystals demonstrate an exceptional photocatalytic production capacity of acetophenone (235 mmol∙g-1), which is 16 times higher than that of pure TiO2 nanocrystals. This work demonstrates the great potential of developing photochromic catalysts for high-efficient ethylbenzene oxidation.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"108 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819035","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Geometric and Electronic Perspectives on Dual-Atom Catalysts for Advanced Oxidation Processes 高级氧化过程中双原子催化剂的几何和电子观点
IF 7 1区 化学
Inorganic Chemistry Frontiers Pub Date : 2025-04-10 DOI: 10.1039/d5qi00478k
Bofan Zhang, Jialiang Rui, Ye Zhang, Luyu Yang, Shiro Kubuki, Yang-Chun Yong, Liang Zhang
{"title":"Geometric and Electronic Perspectives on Dual-Atom Catalysts for Advanced Oxidation Processes","authors":"Bofan Zhang, Jialiang Rui, Ye Zhang, Luyu Yang, Shiro Kubuki, Yang-Chun Yong, Liang Zhang","doi":"10.1039/d5qi00478k","DOIUrl":"https://doi.org/10.1039/d5qi00478k","url":null,"abstract":"With the escalating global challenges of energy scarcity and environmental pollution, the development of efficient and sustainable catalytic technologies has become imperative. Dual-atom catalysts (DACs) have garnered considerable interest, particularly in various catalytic process, demonstrating exceptional promise in enhancing reaction efficiency and selectivity. Unlike prior reviews that primarily emphasize specific or one single reaction process, this review provides a systematic and comprehensive analysis of DACs across diverse oxidation chemistry, including ozone oxidation, Fenton-like reactions, photo/electro/piezo-catalysis, and enzyme-mimetic oxidation. It begins with a concise overview of the discovery, development, and evolution of DACs, alongside a profound investigation of diverse synthesis strategies and state-of-the-art characterization techniques. Moreover, the remarkable improvement of DACs in catalytic process delves into how the geometric microstructure and electronic configuration of DACs including charge transfer, coordination environment, spin state, influence catalytic kinetics and thermodynamics, exploring the relationships between structural geometry, electronic interactions, and catalysis mechanisms. By integrating these multidimensional insights, the review expands conventional paradigms in DACs development and identifies innovative pathways for linking microstructure and catalysis mechanism. Finally, it also emphasizes critical research gaps and emerging opportunities of DACs that warrant further exploration and attention. This review would provide valuable guidance and foundational in rapidly evolving field of DACs.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"39 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813728","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Nanocluster-regulated porous ionic rotaxane assemblies with solvent-adaptability for selective adsorption and conductivity 具有选择性吸附和导电性溶剂适应性的纳米簇调控多孔离子轮烷组件
IF 7 1区 化学
Inorganic Chemistry Frontiers Pub Date : 2025-04-10 DOI: 10.1039/d5qi00535c
Jiaxu Wang, Mingfeng Wei, Zexi Zhu, Bao Li, Lixin Wu
{"title":"Nanocluster-regulated porous ionic rotaxane assemblies with solvent-adaptability for selective adsorption and conductivity","authors":"Jiaxu Wang, Mingfeng Wei, Zexi Zhu, Bao Li, Lixin Wu","doi":"10.1039/d5qi00535c","DOIUrl":"https://doi.org/10.1039/d5qi00535c","url":null,"abstract":"Porous supramolecular assemblies are increasingly recognized for the capabilities in mass transfer and selective loading and release. In this study, a dicationic cyclodextrin[3]rotaxane was synthesized to exhibit adaptivity in the flexible motion between the macrocycle and axle, allowing dynamic structural adjustment during their coassembly with polyanionic nanoclusters. Meanwhile, the anions regulate the assembly to form layered, fibrous, and porous structures. By simply mixing the charged components in solution, the porous ionic rotaxane-cluster assemblies have been prepared, showing selective adsorption and adaptive structural transformations. These assemblies exhibit a \"breathing\" effect in response to solvent adsorption/desorption, thereby enabling ABE mixture separation. DMSO disrupts hydrogen bonds and ionic interactions, allowing recrystallization to form a porous structure with larger pores. This transition is reversible by returning to the original structure in aqueous solution. The reorganization can change proton conductivity by about three orders between the two structures.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"12 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813676","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Doubly Crossed Supercoils Built by Cooperative Anion and Metal Coordination 阴离子与金属配合构建双交叉超级线圈
IF 7 1区 化学
Inorganic Chemistry Frontiers Pub Date : 2025-04-10 DOI: 10.1039/d5qi00611b
Wei Zhao, Hongfei Li, Xinyu Lian, Cheng Jin, Di Meng, Boyang Li, Xiao-Yan Zheng, Xiao-Juan Yang, Biao Wu
{"title":"Doubly Crossed Supercoils Built by Cooperative Anion and Metal Coordination","authors":"Wei Zhao, Hongfei Li, Xinyu Lian, Cheng Jin, Di Meng, Boyang Li, Xiao-Yan Zheng, Xiao-Juan Yang, Biao Wu","doi":"10.1039/d5qi00611b","DOIUrl":"https://doi.org/10.1039/d5qi00611b","url":null,"abstract":"Supercoiled structures with multiple, continuous “figure-eight” conformations, such as complex DNA plectonemes, are ubiquitous and play vital roles in biological systems. In comparison, synthetic small-molecule supercoils with two or more crossings are scarce. Herein, we report a supercoiled plectoneme structure with two crossings assembled by the synergistic cation and anion coordination to a heterotopic ligand, which contains an oligourea backbone for sulfate anion coordination and two pyridyl ends for platinum(II) ion coordination. The supercoiling structure is confirmed by single-crystal diffraction to be a racemic mixture with positive and negative crossings. Enantiopure supercoils can be induced by adenosine monophosphate or inosine monophosphate binding inside the apical loops, resembling the polymerase encapsulation in bacterial plectonemes that guides the DNA and RNA synthesis.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"90 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813839","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Boosting hydrogen evolution and triiodide reduction via electronic coupling on (1T, 2H) MoS2/N-doped carbon dodecahedron (1T, 2H) MoS2/ n掺杂碳十二面体上的电子耦合促进氢的析出和三碘化物的还原
IF 7 1区 化学
Inorganic Chemistry Frontiers Pub Date : 2025-04-09 DOI: 10.1039/d5qi00437c
Lan Yu, Chengxu Liu, Li Sun, Wei Kan, Ying Xie, Xiuwen Wang, Yuying Cao, Bing Zhao, Chunmei Lv
{"title":"Boosting hydrogen evolution and triiodide reduction via electronic coupling on (1T, 2H) MoS2/N-doped carbon dodecahedron","authors":"Lan Yu, Chengxu Liu, Li Sun, Wei Kan, Ying Xie, Xiuwen Wang, Yuying Cao, Bing Zhao, Chunmei Lv","doi":"10.1039/d5qi00437c","DOIUrl":"https://doi.org/10.1039/d5qi00437c","url":null,"abstract":"Designing a noble-metal-free catalyst with desired composition and structure is highly significance for accelerating catalytic kinetics of the hydrogen evolution reaction (HER) and triiodide reduction reaction (IRR), which is essential for advancing green hydrogen production from water electrolysis and improving the power convention efficiency (PCE) of dye-sensitized solar cells (DSSCs). Herein, the small-sized (1T, 2H) phase MoS2 nanosheets were uniformly wrapped around N-doped C dodecahedron (MoS2@NC) through a continuous synthesis strategy with ZIF-8 serving as the original template. When MoS2@NC is used as a catalyst for HER, it only requires a low overpotential of 93 mV to reach 10 mA cm−2, surpassing most reported MoS2-based catalyst. Furthermore, a device fabricated with MoS2@NC achieves a PCE of 8.20%, which is comparable to that of Pt-based ones (8.59%). Theoretical calculation revealed that the enhanced HER activity of MoS2@NC is mainly attributed to the enhanced water adsorption energy and a reduced energy barrier for overcoming the rate-determining step during HER process. Additionally, the interfacial S sites in MoS2@NC are responsible for the excellent catalytic activity in IRR. The experimental and theoretical results collectively confirm that the as-designed MoS2@NC is a promising bifunctional catalyst.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"6 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806312","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Design of an Inflorescence-Type Phosphorus-doped (Ni,Co)–Molybdate Architecture with an Atomically Thin Cobalt Oxide Layer for High-Efficiency Energy Storage Systems 为高效储能系统设计带有原子级氧化钴薄层的花序型掺磷(Ni,Co)钼酸盐结构
IF 7 1区 化学
Inorganic Chemistry Frontiers Pub Date : 2025-04-09 DOI: 10.1039/d5qi00355e
Sangeeta Adhikari, Amarnath T. Sivagurunathan, Do-Heyoung Kim
{"title":"Design of an Inflorescence-Type Phosphorus-doped (Ni,Co)–Molybdate Architecture with an Atomically Thin Cobalt Oxide Layer for High-Efficiency Energy Storage Systems","authors":"Sangeeta Adhikari, Amarnath T. Sivagurunathan, Do-Heyoung Kim","doi":"10.1039/d5qi00355e","DOIUrl":"https://doi.org/10.1039/d5qi00355e","url":null,"abstract":"High-performance asymmetric supercapacitors (ASCs) need to promote the diffusion of the electrolyte into the electrode, a process that is governed by the electron transfer kinetics and morphology of the electrode material. In line with this, the present study designed a phosphorus (P)-doped (Ni,Co)-MoO4 electrode with an inflorescence-like architecture on a central stem and an atomically thin coating of Co3O4 to improve the electron conductivity of the resulting electrode. This unique structure was prepared using a three-step process that included hydrothermal processing, phosphorylation, and the atomic layer deposition of Co3O4. The presence of P in (Ni,Co)-MoO4 caused the Mo to shift to a lower oxidation state, which improved the surface redox behavior of the material. Additionally, the formation of Ni2P and CoP3 nanoparticles on the surface of inflorescence architecture via nanoscale Kirkendall effect boosts the charge storage behavior in the electrode system. As a result, the optimized P-doped (Ni,Co)-MoO4 electrode with a 7 nm layer of Co3O4 (NCMP-7Co) achieved a high specific capacity of 2374 C/g at a current density of 2 A/g with 79.8% capacity retention after 5000 cycles at 10 A/g current density. The mechanism for the optimized electrode based on electrochemical analysis indicates a dominant diffusion-governed behavior. On the other hand, postmortem analysis revealed diffusion of P and Mo from the electrode material with significant structural change. An ASC constructed device with reduced graphene oxide displays fairly high energy density compared to reported systems. Convincingly, a synergistic improvement with outstanding performance could be owed to the inflorescence flower-like architecture, compositional arrangement after P-doping, and deposition of the Co3O4 atomic layer.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"1 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806314","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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