Inorganic Chemistry Frontiers最新文献

{"title":"Realizing Efficient Broadband Near-Infrared Emission under Blue Light Excitation in Sb3+-Doped Zero-Dimensional Organic Tin(IV)-Based Metal Halides via Coordination Structure Modulation","authors":"Bao Ke, Hui Peng, Yongqi Yang, Chengzhi Yang, Shangfei Yao, Arfan Bukhtiar, Qilin Wei, Jialong Zhao, Bingsuo Zou","doi":"10.1039/d4qi01904k","DOIUrl":"https://doi.org/10.1039/d4qi01904k","url":null,"abstract":"Realizing Sb3+-activated efficient broadband near-infrared (NIR) emission under blue light excitation remains a significant challenge in lead-free metal halides. To overcome the above difficulties, a coordination structure modulation strategy was adopted, and the broadband NIR emission under blue light excitation was achieved in Sb3+-doped zero-dimensional (0D) organic tin(IV) bromide. Compared to the weak visible light emission with a photoluminescence quantum yield (PLQY) of 2.4% for pure (TBP)2SbBr5 (TBP = Tetrabutylphosphonium), Sb3+-doped (TBP)2SnBr6 exhibits efficient broadband NIR emission band at 705 nm with PLQY of 33.2% upon 452 nm excitation, which stems from self-trapped exciton emission. Combined with experiments and theoretical calculations, we find that the large excited-state lattice distortion degree compared to the ground state and the narrow bandgap are dominant reasons for Sb3+-doped (TBP)2SnBr6 shows efficient NIR emission under blue light excitation. More particularly, Sb3+-doped (TBP)2SnBr6 also has excellent anti-water stability, existing stably in water for more than 4 hours while maintaining high luminous efficiency. Based on the excellent stability and unique optical properties of Sb3+-doped (TBP)2SnBr6, a high-performance NIR light-emitting diode (LED) was fabricated by combining a commercial blue LED chip, and its application in night vision was demonstrated.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321844","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}

{"title":"Tetranuclear-cluster-based MOF with low-polar pore environment for efficient C2H6/C2H4 separation","authors":"Meng Feng, Jiantang Li, Xirong Wang, Jingyu Wang, Dongmei Wang, Banglin Chen","doi":"10.1039/d4qi01685h","DOIUrl":"https://doi.org/10.1039/d4qi01685h","url":null,"abstract":"Removing trace ethane (C<small>₂</small>H<small>₆</small>) from ethylene (C<small>₂</small>H<small>₄</small>) to obtain high-purity C<small>₂</small>H<small>₄</small> is of great industrial significance. However, the construction of C<small>₂</small>H<small>₆</small>-selective metal-organic frameworks (MOFs) remains challenging, mainly because C<small>₂</small>H<small>₄</small> has a small dynamic diameter and a large quadrupole moment. It has been reported that ultramicroporous MOFs with tailored pore sizes and weakly polar pore environment can effectively purify C<small>₂</small>H<small>₄</small> from C<small>₂</small>H<small>₆</small>-C<small>₂</small>H<small>₄</small> mixtures. For this purpose, we successfully designed and synthesized one novel MOF material ZJNU-400 with non-polar pore environment. The channel size of ZJNU-400 is equivalent to the size of the C<small>₂</small>H<small>₆</small> molecule, which can provide a more accessible channel surface for C<small>₂</small>H<small>₆</small>. The pore environment of ZJNU-400 is rich in low-polarity aromatic groups, and uncoordinated N and O atoms can interact strongly with C<small>₂</small>H<small>₆</small> molecules. Therefore, ZJNU-400 exhibits significant C<small>₂</small>H<small>₆</small>/C<small>₂</small>H<small>₄</small> (50/50) selectivity (2.82) and C<small>₂</small>H<small>₆</small> uptake (64.3 cm<small>³</small> g<small>^-1</small>) at 298 K and 1 bar, which is superior to many C<small>₂</small>H<small>₆</small>-selective adsorbents. Breakthrough experiment shows that ZJNU-400 can purify C<small>₂</small>H<small>₄</small> from C<small>₂</small>H<small>₆</small>/C<small>₂</small>H<small>₄</small> mixture in one step. GCMC and DFT calculations further revealed that the multiple synergistic interactions between the MOF and C<small>₂</small>H<small>₆</small> enable efficient separation of the C<small>₂</small>H<small>₆</small>-C<small>₂</small>H<small>₄</small> mixture. These results indicate that ZJNU-400 is a promising adsorbent for C<small>₂</small>H<small>₆</small>/C<small>₂</small>H<small>₄</small> separation.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142313884","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}

{"title":"Selective and Catalytic Conversion of Hydroxymethyl Cytosine to Formyl Cytosine by a Synthetic Model of TET Enzymes","authors":"Dipanwita Palit, Debasish Manna","doi":"10.1039/d4qi01965b","DOIUrl":"https://doi.org/10.1039/d4qi01965b","url":null,"abstract":"The TET enzymes, known as the ten-eleven translocation enzymes, have become central figures in epigenetic regulation due to their remarkable ability to oxidize 5-methylcytosine (5-mC) to 5-hydroxymethylcytosine (5-hmC), 5-formylcytosine (5-fC), 5-carboxy cytosine (5-caC) thus influencing gene expression and DNA methylation patterns. Understanding the intricate mechanisms underlying TET enzyme function is crucial for unraveling epigenetic regulatory pathways and their implications in various biological processes, including development, differentiation, and disease progression. Recently, we have shown that FeIIITAML complex acts as a synthetic model of TET enzyme by selectively oxidizing 5-hmC to 5-fC. Herein we report another synthetic model, FeIIIbTAML, for selective and catalytic oxidation of 5-hmC. The current synthetic model overcomes several limitations of the previous TET model reported by us. In addition to oxidizing simple nucleobase, we have shown that the FeIIIbTAML, in the presence of H2O2, can selectively oxidize nucleoside and small DNA fragments containing 5-hmC in a catalytic manner.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142313885","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}

{"title":"Large ferroelectricity in Hf0.85Ce0.15O2−δ polycrystalline thin films via lattice expansion","authors":"Hangren Li, Jie Tu, Guoqiang Xi, Xiuqiao Liu, Xudong Liu, Siyuan Du, Dongfei Lu, Da Zu, Yuxuan Zhang, Qingxiao Wang, Dongxing Zheng, Xixiang Zhang, Jianjun Tian, Linxing Zhang","doi":"10.1039/d4qi01558d","DOIUrl":"https://doi.org/10.1039/d4qi01558d","url":null,"abstract":"The discovery of ferroelectricity in HfO<small>₂</small>-based thin films has strongly energized the field of integrated semiconductor devices. To expand the physical applications of HfO<small>₂</small>-based thin films, it is essential to urgently enhance their ferroelectric polarization. In this work, we have synthesized Hf<small>_0.85</small>Ce<small>_0.15</small>O<small>_{2−<em>δ</em>}</small> thin films with a large remanent polarization of 2<em>P</em><small>_r</small> ∼ 69 μC cm<small>⁻²</small>, which is the maximum of all HfO<small>₂</small>-based polycrystal thin films. The strong increase of the remanent polarization is caused by the significant lattice expansion triggered by the increase of Ce<small>³⁺</small> content, which is controlled by temperature. Due to the increase of the lattice constant in the <em>c</em>-axis, the unit-cell volume expands from 132.16 Å<small>³</small> to 137.66 Å<small>³</small>, inducing an increase in the distortion of ions along the direction of the polarization axis and leading to an increase in polarization. This finding is of significant practical importance for promoting HfO<small>₂</small>-based materials and their development in physical fields.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142277063","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}

{"title":"A General Metal Acetate-Assisted Alcohol Thermal Strategy to Fabricate Flexible Carbon Nanofiber Film for Supercapacitor","authors":"Wei Song, Kaixuan Wang, Xiao Lian, Fangcai Zheng, Chunyan Xu, Helin Niu","doi":"10.1039/d4qi02004a","DOIUrl":"https://doi.org/10.1039/d4qi02004a","url":null,"abstract":"Flexible carbon nanofiber film (CNF) has drawn tremendous attention recently due to their fascinating properties. However, CNF prepared by conventional methods is fragile and easily broken. Therefore, a general approach for synthesizing flexible CNF is urgently needed. Herein, we report a metal acetate-assisted alcohol thermal (MAA) method for the preparation of flexible CNF. The MAA is a general and scalable method which can overcome the shortcomings of the pre-oxidation method, and more than 15 different flexible CNFs are successfully prepared. In this method, polyacrylonitrile (PAN) film is first prepared through an electrostatic spinning process, and then cyclized polyacrylonitrile (CPAN) film with high-temperature-resistant trapezoidal structure is formed after MAA treatment. The unique structure of CPAN will help in maintaining its flexibility to produce flexible CNF during carbonization at elevated temperature. To explore their potential in flexible devices, a supercapacitor made of flexible CNF-Zn is investigated, it shows an energy density of 11.5 Wh kg-1 at 500 W kg-1, and has a capacitance retention rate of 97.2% even after 10,000 charge-discharge cycles. Our findings demonstrate that the MAA method could not only prepare flexible CNF for energy storage devices, and it also has potential application prospects in other fields.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276094","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}

{"title":"Atomically Precise Ag25(SR)18 Nanoclusters: A Steady Photosensitizer for Photocatalysis","authors":"Linjian Zhan, Junyi Zhang, Boyuan Ning, Yunhui He, Guangcan Xiao, Zhixin Chen, Fangxing Xiao","doi":"10.1039/d4qi01976h","DOIUrl":"https://doi.org/10.1039/d4qi01976h","url":null,"abstract":"Atomically precise metal nanoclusters (NCs) served as photosensitizers in photocatalysis have garnered enormous attention due to the quantum confinement effect, unique atom stacking fashion, and enriched catalytic active sites, which makes them promising photosensitizers for solar energy conversion. However, current woks on metal NCs-based photocatalytic systems are still in the infant stage, owing to the complex synthetic strategies of metal NCs and deficiency of metal NCs with favorable energy level configuration, which substantially limit the exploration of metal NCs photocatalytic systems with photocatalytic mechanism remaining elusive. Herein, we conceptually demonstrate the construction of metal NCs/transition metal chalcogenides (TMCs) binary heterostructure photosystem via electrostatic self-assembly under ambient conditions, wherein Ag25(SR)18 NCs (SR: 2,4-dimethylbenzenethiol) are precisely and uniformly anchored on the surface of TMCs and function as light-harvesting antenna. We ascertain that advantageous charge transfer between TMCs and Ag25(SR)18 NCs results in the prolonged the charge lifetime and increased the carrier density. Therefore, self-assembled metal NCs/TMCs heterostructures demonstrate the significantly improved and versatile photoactivities toward the anaerobic photoreduction of aromatic nitro compounds to amino derivatives and heavy metal ions (Cr6+) reduction under visible light. Our work would clarify the photocatalytic mechanism of atomically precisely metal NCs photocatalysis and open new chances for smartly mediate charge transfer and separation of metal NCs toward solar energy conversion.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276096","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}

{"title":"PMMA-Assisted Electrospinning Uniformly Incorporates Magnetic Particles into a Carbon Nanomaterials for Efficient Microwave Absorption","authors":"Xin Kou, Xijin Zhao, XinYao Xiong, Shenglin Yuan, Hui Huang, Yongpeng Zhao, Xiangcheng Li","doi":"10.1039/d4qi02100b","DOIUrl":"https://doi.org/10.1039/d4qi02100b","url":null,"abstract":"The development of magnetic-electric synergistic microwave absorbing materials represents a pivotal strategy for optimizing impedance matching, overcoming skin effects, and enhancing absorbing performance. Achieving a uniform distribution of magnetic particles within the dielectric material during the preparation process poses an immense challenge. In this study, PMMA-assisted electrospinning was employed to achieve a homogeneous dispersion of magnetic particles on the surface of 1D or 2D carbon nanomaterials. The electrospinning process effectively blends the precursor of the magnetic material with the carbon nanomaterials while utilizing PMMA as a sacrificial template to anchor and evenly disperse the magnetic particles onto the carbon material's surface. As anticipated, this approach ensures uniform modification of magnetic particles within the carbon matrix, thereby achieving ideal interface uniformity. Comparative analysis reveals that optimized samples incorporating carbon nanotubes and graphene exhibit significantly reduced minimum reflection loss by 294% and 313%, respectively, compared to those without undergoing electrospinning treatment. Further examination of composite microstructure and electromagnetic parameters underscores that excellent dispersion of magnetic particles is crucial in improving impedance matching. The present article presents a controllable and easily scalable preparation method for constructing interface-uniform dielectric-magnetic composite structures with exceptional homogeneity.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276097","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}

{"title":"H/OH substitution achieving high-temperature multiferroicity in a Sn(Ⅳ)-based hybrid perovskite","authors":"Mei-Ling Ren, Wang Luo, Ze-Jiang Xu, Hua-Kai Li, Lang Liu, Chao Shi, Na Wang, Heng-Yun Ye, Le-Ping Miao","doi":"10.1039/d4qi01301h","DOIUrl":"https://doi.org/10.1039/d4qi01301h","url":null,"abstract":"Organic-inorganic hybrid perovskites (OIHPs) have always been regarded as great potential platforms for obtaining ferroicity due to their easy structural tunability and derivativity. However, compared with the common halogen substitution, there is still a lack of understanding of ferroelectricity design through H/OH substitution. Herein, based on a Sn(Ⅳ)-based OIHP [1, (Piperidinium)2SnCl6], hybrid multiferroic crystal 2 [(R-3-OH-Piperidinium)2SnCl6] and 3 [(S-3-OH-Piperidinium)2SnCl6] were obtained by H/OH substitution on the organic component. Besides, where 3 has a high Curie temperature (Tc) 401 K and a spontaneous polarization (Ps) of 3.62 µC cm‒2, accompanied by a significant dielectric response and second harmonic generation (SHG) switching. The experimental results and molecular structural analysis reveal that ferroelectricity is mainly attributed to the homochirality group. Our work provides deep insight into the design of multiferroic materials and ferroelectric performance optimization at the molecular level.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276095","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}

{"title":"Stabilization of Copper Iodide Hybrids with Increased Strength of Ionic Bonding for Lighting and X-ray Imaging","authors":"Qianqian Wang, Haibo Li, Jiali Fan, Zhennan Zhou, Hua Tong, Jialin Zhu, Wei Liu, Gangfeng Ouyang","doi":"10.1039/d4qi02068e","DOIUrl":"https://doi.org/10.1039/d4qi02068e","url":null,"abstract":"A new strategy of improving the stability of organic-inorganic hybrid materials by increasing the charge of organic compounds to enhance the strength of ionic bonds has been demonstrated. Based on this method, we have designed and synthesized a series of ionic copper iodide hybrid structures with significantly improved stability and excellent photo/radio-luminescence, showing potential as new solid-state lighting phosphors and X-ray scintillators.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276098","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}

{"title":"Engineered iron-doped MOF Nanosheets: Acid-induced lattice strain for enhanced rate performance in asymmetric supercapacitor","authors":"Yuan Yuan, Gong Chen, Qihui Zhao, Yuanzun Fu, Yunhe Zhao","doi":"10.1039/d4qi01670j","DOIUrl":"https://doi.org/10.1039/d4qi01670j","url":null,"abstract":"The development of electrode materials is the key to realizing efficient energy storage. In order to solve the problems of low conductivity and poor cycling stability of existing metal-organic framework (MOF), element doping and chemical etching strategies are effective strategies. In this work, we propose a strategy to modify the surface of MOF via Fe doping and HCl etching strategy. The Jahn-Teller effect was induced and the electronic configuration of Co was optimized by doping Fe3+ ions with [Fe(CN)6]3-. In addition, HCl etching induces lattice strain, enhances the interaction between Fe and Co, and provides a fast charge transfer rate. This synergistic effect enhances the conductivity of Co MOF, introduces more electrochemical active sites, and further accelerates the electrochemical reaction kinetics. In particular, the specific capacity of e-Fe-MOF CNs-30 at 1 A g-1 is as high as 1431 C g-1, and the capacity retention rate is 84.2%. Additionally, the e-Fe-MOF CNs-30//AC asymmetric supercapacitor was assembled, which has a high energy density of 83.75 Wh kg-1 and superior cycling stability of about 91.66% after 5000 cycles. These MOF structural design significantly improve the low energy density and cycle life of MOFs-based supercapacitors and provide insights into the electronic structure regulation and lattice strain engineering of low conductivity MOF electrodes.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":null,"pages":null},"PeriodicalIF":7.0,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142276100","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}