SOLAR ENERGY MATERIALS AND SOLAR CELLS
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2024
·
IF 6.3
Ziqiang Cheng,Gang Xu,Yong Liu,Gaorong Han
Benefitting from large-sized ion tunnels and stable crystalline structures, hexagonal WO 3 (h-WO 3 ) is a promising electrochromic (EC) material. However, long reaction times and highly controlled reaction conditions for preparation hinder the practical application. Here, a novel method with a simple process and moderate condition, named topotactic layer-to-tunnel crystallization (TLTC), to prepare h-WO 3 films is reported. The hexagonal tunnel structure is transformed from a layered structure by annealing, assisted by the structure director. The ACTEM with atomic resolution reveals the position of the structure director in the crystal lattice, which is left in the hexagonal tunnel. The mechanism of TLTC has been studied by the characterization of samples at different formation stages, and the key is the structure director, which maintains the hexagonal tunnel by steric effect. The prepared h-WO 3 film exhibits significant optical modulation (65.8 % at 633 nm and 72.8 % at 1200 nm) and outstanding cyclic stability (98.1 % of initial optical modulation remained over 600 cycles). The TLTC method is based on the structure transition to construct large tunnels in lattice, providing a new technical route to prepare h-WO 3 and showing great potential for EC materials manufacturing.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Hu Yaqi,Liu Runze,Lu Kaiyun,Wu Daoning,Gao Pan,Hou Guangjin,Zhang Hongbo,Dai Weili
Hydrated hydronium ions formed in the pores/cages of zeolite catalysts are suggested as the active species that could impact the adsorption of reactant, the stability of intermediates or transition states, and the reaction mechanism in the aqueous phase alcohol dehydration. Nevertheless, under a typical vapor phase reaction condition, the relevant situation is still debatable. Herein, the promotion of water on cyclohexanol (CyOH) adsorption and dehydration under a vapor phase condition was clarified by in situ 1 H MAS NMR, 2D 1 H DQ MAS NMR and 2D 1 H- 27 Al HMQC NMR spectroscopy, systematic kinetic studies, isotope tracing and thermodynamic measurements. The water promoting effects were ascribed to water facilitating the formation of H 3 O + cluster (H 3 O + (H 2 O) n-1 ), and per Brønsted acid site (BAS) could be saturated by about 5 water at ambient temperature. The CyOH dehydration pathway was found to be highly dependent on the water concentrations, and a dimer reaction route with the C-H bond rupture as the kinetically relevant step (KRS) was verified as the main reaction pathway at high water concentrations. All these findings provide the deep insights into how water regulating the zeolite catalyzed dehydration reaction at a molecular level.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Ligang Ma,Yihuan Ding,Chao Lin,Yuqing Yang,Le Xu,Hui Qiu,Huilin Jiang,Xiang Song,Xiaoqian Ai
The photo-corrosion issue inherent in metal sulfide semiconductors is quite pronounced, making the enhancement of electron-hole pair separation efficiency in these photocatalysts a pivotal strategy for boosting photocatalytic hydrogen production. This study introduces a novel approach where hexagonal boron nitride ( h -BN) acts as a substrate for the in situ growth of ZnIn 2 S 4 nanostructures, resulting in the formation of h -BN@ZnIn 2 S 4 (BN@ZIS) nanocomposites. The electronegativity of h -BN nanosheets is harnessed to facilitate the recombination or electrostatic attraction of photogenerated holes in the ZnIn 2 S 4 photocatalyst. This strategy effectively promotes the separation of photogenerated electron-hole pairs, which is crucial for enhancing photocatalytic performance. The microstructure, morphology and optical properties of BN@ZIS nanocomposites were meticulously investigated. The findings reveal that the incorporation of h -BN nanosheets loads to a more uniform dispersion of the ZnIn 2 S 4 nanostructure, which not only increases the specific surface area but also fosters a tight heterojunction interface between h -BN and ZnIn 2 S 4 . In conclusion, the photocatalytic hydrogen production capabilities of the BN@ZIS nanocomposites were rigorously evaluated. Pure h -BN lacks photocatalytic hydrogen production activity. Conversely, the optimized BN@ZIS composite demonstrated a remarkable enhancement, exhibiting a photocatalytic efficiency that is 9.65 times greater than that of pristine ZnIn 2 S 4 . Furthermore, a plausible mechanism by which BN@ZIS augments photocatalytic hydrogen production has been proposed. This strategy, leveraging the synergistic interaction between h -BN and ZnIn 2 S 4 , is anticipated to be applicable to other semiconductor systems, opening avenues for the advancement of photocatalytic technologies.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-19
·
IF 15.7
Peng Han,Xu Qikui,Zhang Ting,Zhu Jiakai,Pan Jinheng,Guan Xiaoyu,Feng Shan,Wu Jianping,Hu Qi
Lipid droplets (LDs) are the main cellular storage sites for triacylglycerols (TAGs), playing an important role in energy homeostasis and cell signaling. Hydrolysis of the stored TAGs begins with conversion of TAGs into diacylglycerols (DAGs) by adipose triglyceride lipase (ATGL), followed by hydrolysis of DAGs by hormone-sensitive lipase (HSL). Despite the central role of HSL in lipolysis, the molecular determinants for its LD association have remained elusive. Here, we report the cryo-EM structure of human HSL at 3.4 Å. Combining this with hydrogen-deuterium exchange mass spectrometry, biochemical and cellular assays, we identify residues 489-538, referred to as the “H-motif”, and the N-terminal 4-helix bundle of HSL as LD-binding motifs mediating direct interaction of HSL with LDs. LD binding mediated by the LD-binding motifs is independent of HSL phosphorylation catalyzed by the cAMP-dependent kinase PKA. Our findings provide insight into the LD binding mechanism of HSL, advancing our understanding of the regulation of lipolysis.
研究领域:
分子生物学
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细胞生物学
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结构生物学
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Chen Cai,Jiayin Chen,Wei Fu,Shuying Ning,Hao Zhou,Muhammad Kashif,Yaxin Su
The Ce-modified OMS-2 catalyst (Ce x -OMS-2) was synthesized by the hydrothermal synthesis method, after which its catalytic efficacy in the selective reduction of NO by CO was assessed. The experiments showed that Ce 0.08 -OMS-2 was capable of 100% NO conversion between 175 and 300 °C when 0.05%NO, 0.1%CO, 5%O 2 and N 2 were used as equilibrium gases, and the N 2 selectivity peaked at 93.2% at 175 °C. Additionally, Ce 0.08 -OMS-2 exhibits good sulfur resistance in the presence of 0.02% SO 2 and maintains more than 88% NO conversion at 175–275 °C. By using BET, XPS, H 2 -TPR, NH 3 -TPD, and In situ DRIFTS to characterize the catalysts, the effects of doping the active metal Ce on the physicochemical characteristics of OMS-2 catalysts were under investigation. In conclusion, the improvement of the low-temperature activity of the Ce x -OMS-2 catalyst is facilitated by lower agglomeration and crystallinity , larger specific surface area, smaller average pore size, enhanced surface oxygen vacancies, increased Mn 4+ concentration, and richer Brønsted acid. Reaction gas adsorbed species and intermediates on the catalyst surface were dynamically captured during In situ DRIFTS experiments. The CO-SCR reaction of the catalyst was found to follow the E-R mechanism below 200 ℃ and the L-H mechanism at 200–350 ℃.
研究领域:
环境科学
·
催化化学
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Kaifu Lin,Jiawei Wang,Shujie Qiao,Zhiyong Guo
As one of the most direct methods to construct molecular scaffolds in fine chemicals, C–H bond oxidation is a hot research area in catalysis. One-dimensional covalent organic frameworks (1D-COFs) developed recently have attracted growing attention for catalytic applications owing to their unique edge microstructure. Herein, a novel crystalline 1D-COF (FZU-66) was constructed and further decorated with cobalt(II), which led to excellent heterogeneous catalytic performance in the C–H bond oxidation of ethylbenzene. In an aqueous solution at room temperature within 16 h, the conversion is nearly 100%, while the acetophenone selectivity is around 99%. More impressively, the designed single-dispersed cobalt(II)-coordinated 1D-COF (FZU-66-Co) retained good catalytic activity while maintaining high crystallinity after at least five consecutive recycling experiments. This work will prompt the application of porous polymers in the catalyzed oxidation of C–H bonds and make it an efficient and sustainable platform for activating C–H bonds of aromatic hydrocarbons.
研究领域:
催化化学
·
材料科学
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FUEL
·
2024
·
IF 6.7
Yiran Zhang,Zhiyuan Yuan,Ji Mi,Xufeng Li,Yongsheng Guo,Wenjun Fang
Tetrahydrotricyclopentadiene (THTCPD) is a new high energy–density fuel with a density of 1.05 g·cm -3 and a volumetric net heat of combustion of 44.7 MJ·L -1 , which has an excellent potential for actual use. Thermal oxidation of hydrocarbon fuel is a key issue in application, however, the oxidation performance of THTCPD has not yet been studied. In this work, a comprehensive investigation was conducted for the first time on the thermal oxidation of synthesized THTCPD fuel, including oxidation stability, mechanism and inhibition. The experimental and theoretical results show that the oxidation stability of THTCPD mainly depends on its lowest C−H bond dissociation enthalpy, and the oxidation initially occurs on the symmetrical secondary carbon atoms of the five-membered ring in the molecule, primarily triggered by the cleavage of C−H bonds. In addition, phenolic antioxidants can significantly inhibit the thermal oxidation of THTCPD. Among them, butyl hydroxy anisole exhibits the most effective performance, which can enhance the oxidation stability of THTCPD to be comparable to that of other typical fuels. This work presents a thorough perspective on the thermal oxidation of THTCPD fuel, which is beneficial for its specific application and offers guidance for future research on high energy–density fuels.
研究领域:
化学工程
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能源科学
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材料科学
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JOURNAL OF ORGANIC CHEMISTRY
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2025
·
IF 3.6
Huanhuan Cui,Chunyu Hu,Xiulin Qiao,Tiesheng Shi,Chao Chen,Wei Wei,Zu-Li Wang,Zhuoming Ma
An efficient visible-light-induced EDA strategy has been developed for constructing 3-difluoroalkylated quinoxalin-2(1H)-ones through the C–H difluoroalkylation of quinoxalin-2(1H)-ones with fluoroalkyl bromides. This transformation could provide a series of 3-difluoroalkylated quinoxalin-2(1H)-ones in moderate to good yields under mild and metal-free conditions. Mechanistic studies revealed that the formation of the EDA complex between fluoroalkyl bromide and TMEDA was essential to initiate this transformation.
研究领域:
有机化学
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药物化学
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光氧化还原催化
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PROGRESS IN ORGANIC COATINGS
·
2021
·
IF 5.161
Beibei Chen,Zhe Dong,Jiaye Li,Mengjie Zhang,Kan Zhang
Hexagonal boron nitride (h-BN) is a promising additive used in tribology ; however, its application is limited due to its poor interfacial combination with polymer matrices induced by its inert and smooth surface. In order to tackle this problem, an innovative ZnO nanowires-decorated h-BN hybrid was first prepared, which was then applied onto epoxy (EP) to enhance its tribological properties. The results demonstrated that ZnO nanowires were in-situ grown uniformly on the exterior of the hydroxylated h-BN, which strengthened the physical and chemical interaction between h-BN and EP, since the EP chains were prone to wrap around the ZnO nanowires. When the h-BN/ZnO content was 0.5 wt%, the friction coefficient and wear rate were decreased by 81.5% and 95.4%, respectively, and the corresponding composite coating possessed superior tribological properties under harsh conditions, which was mainly because of the synergistic reinforcing and lubricating effect between the ZnO nanowires and h-BN, as well as the good interfacial compatibility between h-BN/ZnO hybrid and EP. Moreover, the corresponding enhancement mechanisms of h-BN/ZnO were proposed.
研究领域:
材料科学
·
摩擦学
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Hang Che,Yuhao Wu,Xinhua Wang,Haizhen Liu,Mi Yan
The Mg(NH 2 ) 2 -2LiH system is considered as one of the most potential hydrogen storage materials due to its high hydrogen storage capacity (5.6 wt%) and excellent reversible hydrogen adsorption and desorption performance. However, its poor kinetic characteristics of hydrogen absorption and desorption limit its practical application. In this work, Li 3 VO 4 @LiVO 2 was synthesized by a hydrothermal method , and was then introduced into Mg(NH 2 ) 2 -2LiH system to enhance the hydrogen absorption and desorption kinetic characteristics. The results show that the hydrogen storage properties were greatly improved with addition of 10 wt% Li 3 VO 4 @LiVO 2 addition. As for the hydrogen absorption and desorption kinetics, the average hydrogen absorption rate of 10 wt% Li 3 VO 4 @LiVO 2 modified Li-Mg-N-H sample within 20 min at 200 ℃ increased by 95.2% compared with that of the pristine Li-Mg-N-H sample, and the average hydrogen desorption rate of 10 wt% Li 3 VO 4 @LiVO 2 modified sample within 30 min at 180 ℃ increased by 42% compared with that of the pristine sample. The E a of hydrogen desorption decreased from 117.86 kJ/mol to 99.43 kJ/mol, which also indicates that Li 3 VO 4 @LiVO 2 catalyst effectively improved the kinetic performance of hydrogen desorption and desorption of Li-Mg-N-H. Moreover, the hydrogen desorption capacity and hydrogen absorption capacity of 10 wt% Li 3 VO 4 @LiVO 2 modified Li-Mg-N-H increased by 18.4% and 13.8% compared with that of the pristine sample. The catalytic mechanism of Li 3 VO 4 @LiVO 2 was discussed based on XRD , XPS and FTIR analysis results.
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CHINESE JOURNAL OF POLYMER SCIENCE
·
2017
·Vol. 36
·期 3
·406-416
·
IF 1.692
Bai Yang,Xie Fang-Yuan,Tian Wei
Despite the fact that some progress has been made in the self-assembly of H-shaped polymers, the corresponding self-assemblies that respond to external stimulus and are further utilized to adjust the release of drugs are still deficient. The stimuli-responsive segments with amphiphilic H-shaped structure are generally expected to enhance the controllability of self-assembly process. The synthesis and self-assembly behavior of thermo-responsive amphiphilic H-shaped polymers with poly(ethylene glycol) (PEG), polytetrahydrofuran (PTHF) and poly(N-isopropyl acrylamide) (PNIPAM) as building blocks are reported in this paper. The inner architecture structure and size of complex micelles formed by H-shaped self-assemblies were effectively adjusted when the solution temperature was increased above the lower critical solution temperature of PNIPAM segments. Furthermore, it was found that the architecture of self-assemblies underwent a transition from the complex micelles based on primary micelles with hybrid PEG/PNIPAM shells to large complex micelles based on primary micelles with hybrid PTHF/PNIPAM cores and PEG shells during the thermal-induced self-assembly process. The adjustable release rate of doxorubicin (DOX) from the DOX-loaded complex micelles and basic cell experiments further proved the feasibility of these self-assemblies as the thermal-responsive drug delivery system.
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JOURNAL OF ORGANOMETALLIC CHEMISTRY
·
2024
·
IF 2.1
Chao-Chao Teng,Yan Guo,Ke Cao,Han-Bo Yang,Qi-Jia Jiang,Dao-Yong Zhu,Shao-Hua Wang
A palladium catalyzed selective arylation of B(4)-H of 9-amide- o -carborane with potassium aryltrifluoroborate has been developed. A series of B(4)-Ar-B(9)-amide- o -carborane derivatives decorated with diverse active groups have been synthesized with moderate to good yields as well as excellent selectivity. This work represents an unprecedented protocol for selective arylation of o -carboranes with potassium aryltrifluoroborates.
研究领域:
有机化学
·
金属有机化学
·
药物化学
·
材料科学
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危险品化学品经营许可证（带存储）