Inorganic Chemistry Frontiers最新文献_第5页

Insights into Atomic Level Defect Commanding coupling with n-π* Excitation in Carbon Nitride for enhanced photocatalytic Hydrogen Production and CO2 reduction

IF 7 1区化学

Inorganic Chemistry Frontiers Pub Date : 2025-02-04 DOI: 10.1039/d4qi02990a

Shukui Shi, Huibin Zong, Zhimin Yuan, Zaiyong Jiang, Haotian Qi, Zhao Mo, Xianglin Zhu

{"title":"Insights into Atomic Level Defect Commanding coupling with n-π* Excitation in Carbon Nitride for enhanced photocatalytic Hydrogen Production and CO2 reduction","authors":"Shukui Shi, Huibin Zong, Zhimin Yuan, Zaiyong Jiang, Haotian Qi, Zhao Mo, Xianglin Zhu","doi":"10.1039/d4qi02990a","DOIUrl":"https://doi.org/10.1039/d4qi02990a","url":null,"abstract":"The restricted internal charge migration and inadequate light trapping impede the optimization of the intrinsic efficacy of the g-C3N4 photocatalyst. In the present study, efforts were directed towards minimizing the impact of in-plane defects resulting from the N-(C)3 defect site, with the objective of enhancing the efficient rapid separation of charge carriers. Moreover, the incorporation of a C-C bond within the tris-triazine units facilitated n→𝜋* excitation, thereby enhancing the efficiency of light utilization. Consequently, the modified catalyst exhibited markedly enhanced photocatalytic activity under visible light, with an absorption edge extending from 450 to 550 nm. The optimized SCN-5 sample demonstrated notable enhancements in reaction rates for hydrogen production, CO₂ reduction, and pollutant degradation, with factors of 11.0, 4.2, and 14.3, respectively. These improvements can be attributed to the enhanced light trapping and charge separation capabilities of the sample. This research underscores the significance of impeding in-plane defects and fostering local n→𝜋* excitation in order to augment intrinsic visible light catalytic reactions. This provides a vital mechanism for the development of high-performance photocatalysts.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"10 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083636","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

Stabilizing Rh Nanoparticles by TiO2 Array with Oxygen Vacancies for High‐performance pH-wide Hydrogen Evolution

IF 7 1区化学

Inorganic Chemistry Frontiers Pub Date : 2025-02-04 DOI: 10.1039/d4qi03077j

Guangxia Wang, Wenhui Wang, Yaozhong Yu, Tao Hu, Juan Ding, Yongming Sui

{"title":"Stabilizing Rh Nanoparticles by TiO2 Array with Oxygen Vacancies for High‐performance pH-wide Hydrogen Evolution","authors":"Guangxia Wang, Wenhui Wang, Yaozhong Yu, Tao Hu, Juan Ding, Yongming Sui","doi":"10.1039/d4qi03077j","DOIUrl":"https://doi.org/10.1039/d4qi03077j","url":null,"abstract":"Active and durable catalysts are crucial for hydrogen evolution reaction (HER). In the volcano plot, Rhodium (Rh) and Platinum (Pt) are positioned closely, while the activity and stability of Rh are much inferior to Pt. Here, we developed Rh/TiO2/Ti electrocatalyst to mitigate Pt dependency. The in-situ formed TiO2 with oxygen vacancies was prepared utilizing Ti foam as Ti source. TiO2 support can confine Rh nanoparticles and ensure charge accumulation at Rh site, while Rh can enhance the conductivity of TiO2. DFT calculations demonstrate that the strong interaction between Rh and TiO2 could regulate the electronic structure of Rh, thereby accelerating water dissociation and optimizing the adsorption strength of *H. Consequently, compared to Rh/Ti, Rh/TiO2/Ti exhibits significantly enhanced HER activity, requiring only overpotentials of 37.3 and 34.3 mV to reach 10 mA cm−2 in alkaline and acidic HER, respectively. Furthermore, the vertical nanoarrays structure, surface roughness, and metal-support interaction endow Rh/TiO2/Ti remarkable durability. It works in both alkaline and acidic media for 120 hours at 10 mA cm−2 with unnoticeable activity decline, outperforming commercial Pt/C. This work provides a strategy to overcome the activity and stability limitations of Rh-based catalysts, providing references for promising catalysts for water electrolysis.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"10 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083752","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

Fe-doped Ni3S2/NiS heterojunction with improved electrocatalytic activity and stability for the alkaline oxygen evolution reaction

IF 7 1区化学

Inorganic Chemistry Frontiers Pub Date : 2025-02-04 DOI: 10.1039/d4qi02957g

Jiening Sun, Licheng Miao, Zhichuan J. Xu, Zhipeng Sun

{"title":"Fe-doped Ni3S2/NiS heterojunction with improved electrocatalytic activity and stability for the alkaline oxygen evolution reaction","authors":"Jiening Sun, Licheng Miao, Zhichuan J. Xu, Zhipeng Sun","doi":"10.1039/d4qi02957g","DOIUrl":"https://doi.org/10.1039/d4qi02957g","url":null,"abstract":"During the oxygen evolution reaction (OER), Ni-based sulfide catalysts undergo dynamic restructuring under high current operating conditions, which can have a detrimental impact on their activity and stability. In this study, we have developed an Fe-doped Ni3S2/NiS heterojunction catalyst (Fe-Ni3S2/NiS) for the OER that exhibits exceptional durability and activity. The catalyst has demonstrated the ability to operate continuously for 72 h at current densities of 500 and 1000 mA cm−2 without performance degradation in an alkaline electrolyte environment. This catalyst requires an overpotential of only 247 mV to drive the OER at 100 mA cm−2. Experimental results suggest that the doped Fe acts as a sacrificial agent in the OER process, facilitating electron transfer, maintaining the high activity of Ni, and protecting the Ni–S bond from degradation. Theoretical computations further indicate that the doped Fe reduces the OER energy barrier and enhances the intrinsic conductivity of the material, thereby improving catalytic efficiency.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"694 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083751","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

Multidentate chelation via pyridine-based molecules for high-efficiency perovskite solar cells 通过基于吡啶的分子进行多叉螯合，实现高效率的过氧化物太阳能电池

IF 7 1区化学

Inorganic Chemistry Frontiers Pub Date : 2025-02-03 DOI: 10.1039/d4qi03269a

Yongxiang Zhang, Jinfeng Zhang, Aiqin Sun, Zhiqian Yang, Mengting Han, Yang Huang, Mei Lyu, Yan Meng, Jun Zhu, Linhua Hu

{"title":"Multidentate chelation via pyridine-based molecules for high-efficiency perovskite solar cells","authors":"Yongxiang Zhang, Jinfeng Zhang, Aiqin Sun, Zhiqian Yang, Mengting Han, Yang Huang, Mei Lyu, Yan Meng, Jun Zhu, Linhua Hu","doi":"10.1039/d4qi03269a","DOIUrl":"https://doi.org/10.1039/d4qi03269a","url":null,"abstract":"The non-radiative recombination loss at the interface between a perovskite layer and hole transport layer is one of the main sources of energy loss in perovskite solar cells (PSCs). Non-radiative recombination caused by surface defects greatly limits further improvement of power conversion efficiency (PCE). Interfacial passivation is one of the commonly used methods to improve PCE, but traditional passivation methods often involve single-point coordination, and their passivation effect is limited. In this study, we used a multi-site binding passivation method, introducing diethyl 2,6-pyridinedicarboxylate (DIP) as a passivation layer at the interface between the perovskite and the hole transport layer. The ester and pyridinium groups can interact effectively with uncoordinated Pb2+, and this multidentate chelation effect can repair various defects, improve crystallization, and promote interfacial carrier transfer. As a result, the optimized device achieves an efficiency of 23.68%. Additionally, due to the hydrophobicity of DIP, the device exhibits excellent humidity stability, maintaining 89.40% of its initial PCE after 550 hours at a relative humidity of 65 ± 5%.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"36 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077307","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

Engineering tri-channel orthogonal luminescence in a single nanoparticle for Information Encryption

IF 7 1区化学

Inorganic Chemistry Frontiers Pub Date : 2025-02-01 DOI: 10.1039/d4qi03199g

Jianhao Zheng, Pengye Du, Ran An, Yuan Liang, Yi Wei, Shuyu Liu, Pengpeng Lei, Hongjie Zhang

{"title":"Engineering tri-channel orthogonal luminescence in a single nanoparticle for Information Encryption","authors":"Jianhao Zheng, Pengye Du, Ran An, Yuan Liang, Yi Wei, Shuyu Liu, Pengpeng Lei, Hongjie Zhang","doi":"10.1039/d4qi03199g","DOIUrl":"https://doi.org/10.1039/d4qi03199g","url":null,"abstract":"Optical anti-counterfeiting technology based on the multicolor emission generated by the abundant energy levels of rare earth ions shows great potential in the face of increasing information security problems worldwide. However, it is not an easy task to achieve multi-channel orthogonal emissions in a single nanoparticle with simple structure by convenient method. In this work, we have successfully realized the tri-channel orthogonal emissions under three excitation wavelengths in the NaErF4@NaYF4:Eu3+@NaBiF4:Yb3+,Tm3+ core@shell@shell nanoparticles. In our design, the interlayer NaYF4:Eu3+ plays the role of a piece of three carvings. Not only it can enhances the upconversion luminescence intensity of NaErF4, but also makes the emission color of Er3+ changes from red to green by the energy transfer process between Er3+ and Eu3+. Moreover, it can produces red emission under 395 nm light excitation. This selective excitation strategy enables R-G-B tri-channel orthogonal emissions in a single nanoparticle by simply changing the excitation wavelength, which is very suitable for high level optical information encryption. This work provides a simple and effective method for the design of smart luminescent materials, showing great potential for multi-level anti-counterfeiting and information security.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"50 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143071614","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

The X-ray structure of the adduct formed upon reaction of aurothiomalate with apo-transferrin: gold binding sites and a unique transferrin structure along the apo/holo transition pathway

IF 7 1区化学

Inorganic Chemistry Frontiers Pub Date : 2025-01-31 DOI: 10.1039/d4qi03184a

Romualdo Troisi, Francesco Galardo, Luigi Messori, Filomena Sica, Antonello Merlino

引用次数: 0

Novel zinc(II) phthalocyanine nanoparticles as diagnosis-treatment nanoprobe for photoacoustic imaging-guided synergistic photothermal/photodynamic-enhanced cancer therapy

IF 7 1区化学

Inorganic Chemistry Frontiers Pub Date : 2025-01-31 DOI: 10.1039/d4qi02898h

Min He, Yidong Bin, Lixian Huang, Caiying Li, Yuzhen Ma, Yan-Ni Luo, Shulin Zhao, Jinzhe Liang

引用次数: 0

What determines the Th/U atom positions inside fullerenes?

IF 7 1区化学

Inorganic Chemistry Frontiers Pub Date : 2025-01-31 DOI: 10.1039/d4qi03104k

Jilong Chen, Lei Lou, Peng Jin

{"title":"What determines the Th/U atom positions inside fullerenes?","authors":"Jilong Chen, Lei Lou, Peng Jin","doi":"10.1039/d4qi03104k","DOIUrl":"https://doi.org/10.1039/d4qi03104k","url":null,"abstract":"Understanding the exact position of metal atom(s) within cage is critical for elucidating the structural characteristics, metal-cage interplay and stability mechanism of endohedral metallofullerenes (EMFs). But it becomes rather challenging for the emerging actinide EMFs due to the variable oxidation state and complex valence orbitals of the encapsulated metals. Herein, density functional theory calculations were carried out for all 25 reported Th/U-based mono-metallofullerenes (mono-EMFs) with well-defined single crystal structures. The electronic ground states of Th- and U-contained mono-EMFs are singlet and triplet/quintet, respectively. Th always formally assumes the IV oxidation state inside cage, whereas U has the III or IV valence state highly depending on the cage structure. The considerable intramolecular charge transfer (Th: 4e; U: 3e or 4e) results that their metal-cage interactions are mainly ionic, but with non-negligible covalent components largely contributed by the spatially extended Th/U-5f orbitals. Importantly, all the internal Th4+/U3+/4+ cations can be located by only considering the frontier molecular orbital distributions of corresponding empty cages rather than the electrostatic potentials of cage anions commonly used for the classic lanthanide mono-EMFs. Such an obvious deviation from the simple ionic model (Mq+@C2nq-) is ascribed to the strong actinide-cage covalency, which leads to much lower actual metal charge than the formal one. Our work unprecedently finds the overlooked important role of cage orbitals in determining the internal metal positions of all actinide mono-EMFs. It not only demonstrates the uniqueness of actinide EMFs, but also could help understand the structural characteristics of more EMFs with multiple possible internal metal locations.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"22 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143071615","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

Photoactivation of cGAS-STING Pathway and Pyroptosis by Endoplasmic Reticulum-Targeting Ruthenium(II) Complex for Cancer Immunotherapy

IF 7 1区化学

Inorganic Chemistry Frontiers Pub Date : 2025-01-31 DOI: 10.1039/d4qi03021d

Bin-Fa Liang, Shan Jiang, Yun-Shi Zhi, Zheng-Yin Pan, Xiu-Qin Su, Qin Gong, Zhen-Dan He, da hong yao, Liang He, Chen-Yang Li

{"title":"Photoactivation of cGAS-STING Pathway and Pyroptosis by Endoplasmic Reticulum-Targeting Ruthenium(II) Complex for Cancer Immunotherapy","authors":"Bin-Fa Liang, Shan Jiang, Yun-Shi Zhi, Zheng-Yin Pan, Xiu-Qin Su, Qin Gong, Zhen-Dan He, da hong yao, Liang He, Chen-Yang Li","doi":"10.1039/d4qi03021d","DOIUrl":"https://doi.org/10.1039/d4qi03021d","url":null,"abstract":"Three multifunctional ruthenium(II) complexes (Ru1-Ru3) modified with cholic acid, were synthesized, which possessed excellent singlet oxygen-generating ability and near-infrared (NIR) aggregation-induced emission (AIE) phosphorescence activity. Cellular toxicity assays revealed that Ru1 displayed pronounced phototoxicity against both human breast cancer cells (MDA-MB-231) and murine breast cancer cells (4T1), achieving a maximum phototoxicity index (PI) of 86.21. Mechanistic studies indicated that Ru1 possessed superior targeting affinity for the endoplasmic reticulum (ER). Upon irradiation at 450 nm, it stimulated the production of reactive oxygen species (ROS) and initiated ER stress. This stress activated the STING pathway's signaling cascade within the ER, prompting a Golgi apparatus response. The consequent activation induced pyroptosis and sequentially engaged the downstream proteins p-TBK1 and p-IRF3 within the STING pathway, thus promoting the secretion of antitumor cytokines and the elicitation of tumor immune responses. In vivo experiments conducted on Balb/c mice have demonstrated significant anti-tumor immune effects exhibited by Ru1. In summary, the immune modulation and targeted intervention by metal complexes represent an innovative and promising therapeutic strategy for cancer. This approach is anticipated to yield new perspectives for the development of metal complexes that augment tumor immunotherapy.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"36 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143071616","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

A Self-activation Strategy to Prepare ZIF-8 Derived N, O Co-doped Meso-microporous Carbon for Zinc Ion Hybrid Capacitors

IF 7 1区化学

Inorganic Chemistry Frontiers Pub Date : 2025-01-30 DOI: 10.1039/d4qi02657h

Yanyan Wang, Te Huo, Chunxia Chen, Lichao Tan, Lan Wang, Xiaoliang Wu, Xin Wang

{"title":"A Self-activation Strategy to Prepare ZIF-8 Derived N, O Co-doped Meso-microporous Carbon for Zinc Ion Hybrid Capacitors","authors":"Yanyan Wang, Te Huo, Chunxia Chen, Lichao Tan, Lan Wang, Xiaoliang Wu, Xin Wang","doi":"10.1039/d4qi02657h","DOIUrl":"https://doi.org/10.1039/d4qi02657h","url":null,"abstract":"Porous carbon derived from metal-organic frameworks (MOFs) is usually carbonized and then activated by the additional introduction of potassium hydroxide. The use of a large amount of strong alkali during the reactivation process not only corrodes equipment but also pollutes the environment, which is not conducive to large-scale production. Herein, for the first time, we report a novel self-activation strategy of the fabrication of porous carbon derived from zeolitic imidazolate framework-8 (ZIF-8), where the activator ZnCl2 is derived from the pickling step following the initial carbonization of ZIF-8. The optimized porous carbon (ZPC-800) materials show a high specific surface area with an interconnected micro/mesoporous structure and rich nitrogen (17.3 at.%) and oxygen (9.5 at.%) functional groups. As a result, the assembled Zn//ZnSO4(aq)//ZPC-800 hybrid capacitor achieves a high capacity of 165.2 mAh g-1 and impressive energy/power density of 111.2 Wh kg-1/8.0 kW kg-1. This study provides a new prepare method for the preparation of porous carbon materials for zinc ion hybrid capacitors.","PeriodicalId":79,"journal":{"name":"Inorganic Chemistry Frontiers","volume":"2673 1","pages":""},"PeriodicalIF":7.0,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056940","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