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学者姓名:谢在来
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Harnessing supramolecular interactions to regulate the structure and performance of functional materials is a key challenge in materials chemistry. Herein, the study utilizes 18-crown-6 (18C6) ether-assisted alkali-metal (Na, K, Cs) copper(I) iodide supramolecular assemblies to precisely regulate the material structures. This approach facilitated the transition from 1D mono-royal crown coordination (18C6@KCuI2, CKCI) to 0D di-royal crown ((18C6)(2)@Na-2(H2O)(3)Cu4I6, CNCI) and tri-royal crown ((18C6)(3)@Cs2Cu2I4, CCCI) structures. Interestingly, the CCCI single-crystal exhibits outstanding scintillation properties, with a high relative light yield of 71 000 photons MeV-1 and an ultralow detection limit of 39.3 nGy s(-1), which can be attributed to the synergistic effects of 18C6 and copper-iodide clusters. It stabilizes the self-trapped exciton state, enhances exciton localization, and reduces non-radiative losses, thus resulting in a large Stokes shift of 193 nm and near-unity photoluminescence quantum yield of 99.4%. Additionally, 18C6 can promote crystal nucleation and growth, making it easy to prepare centimeter-scale transparent single crystals with >80% transmittance, such as CCCI single crystal can achieve an ultrahigh-resolution X-ray imaging of 26.3 lp mm(-1). It demonstrates that the structure and performance of halide scintillators can be regulated through supramolecular interactions, which provides a new approach for developing high-performance scintillator materials.
Keyword :
18-crown-6 18-crown-6 copper(I) iodide copper(I) iodide self-trapped exciton state self-trapped exciton state supramolecular scintillators supramolecular scintillators X-ray imaging X-ray imaging
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GB/T 7714 | Ye, Yuanji , Di, Yiming , Zhou, Jiahao et al. Crown Ether-Assisted Alkali-Metal Copper(I) Iodide Supramolecular Scintillators with Near-Unity Emission for Ultrahigh-Resolution X-Ray Imaging [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
MLA | Ye, Yuanji et al. "Crown Ether-Assisted Alkali-Metal Copper(I) Iodide Supramolecular Scintillators with Near-Unity Emission for Ultrahigh-Resolution X-Ray Imaging" . | ADVANCED FUNCTIONAL MATERIALS (2025) . |
APA | Ye, Yuanji , Di, Yiming , Zhou, Jiahao , Qiu, Qiangwen , Chen, Yuhua , Zhong, Shanyuan et al. Crown Ether-Assisted Alkali-Metal Copper(I) Iodide Supramolecular Scintillators with Near-Unity Emission for Ultrahigh-Resolution X-Ray Imaging . | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
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The oxidative dehydrogenation of propane (ODHP) represents a highly promising route for the industrial-scale production of propene. Non-metallic boron nitride (BN)-based materials, known for their high propene selectivity, have emerged as next-generation ODH catalysts. However, the real active sites on surfaces remain unclear due to the absence of visual experimental evidence. In this work, we introduce a chemical titration approach to clarify the active centers of NaOH modified BN (BN-NaOH) catalysts for ODHP. The BN-NaOH catalyst demonstrates outstanding performance, achieving over 90 % olefin selectivity and a stable propane conversion of 23.2 %. Notably, the turnover frequency (TOF) for B-OH sites reaching 1.2 h- 1, which significantly surpassed that of unmodified BN catalysts (0.6 h- 1). In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analysis revealed that the formation of OH-nests on the BN-NaOH surface was primarily accountable for the enhanced reactivity. Moreover, the crucial role of these OH-nests during ODHP was further validated through selective chemical titration of B-OH groups using benzoic anhydride.
Keyword :
Active sites Active sites Boron hydroxyl group Boron hydroxyl group In situ DRIFTS In situ DRIFTS Oxidative dehydrogenation of propane Oxidative dehydrogenation of propane
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GB/T 7714 | Duan, Qiwei , Hu, Zhengli , Hu, Aoxue et al. Identification of active sites in boron nitride for propane oxidative dehydrogenation catalysis [J]. | CHEMICAL ENGINEERING SCIENCE , 2025 , 306 . |
MLA | Duan, Qiwei et al. "Identification of active sites in boron nitride for propane oxidative dehydrogenation catalysis" . | CHEMICAL ENGINEERING SCIENCE 306 (2025) . |
APA | Duan, Qiwei , Hu, Zhengli , Hu, Aoxue , Huang, Shuping , Chen, Ziyi , Yu, Kaihua et al. Identification of active sites in boron nitride for propane oxidative dehydrogenation catalysis . | CHEMICAL ENGINEERING SCIENCE , 2025 , 306 . |
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Glycosyl aryl sulfones exhibit diverse biological activities. Herein, we developed a copper-promoted coupling strategy using glycosyl sodium sulfinates and aryl iodides or bromides, enabling efficient synthesis of carbohydrate-based sulfone with broad functional group compatibility. This method offers a versatile approach for the late-stage modification of bioactive molecules.
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GB/T 7714 | Wang, Linyitian , Guo, Huize , Luo, Jiaxin et al. Copper-promoted late-stage glycosylsulfonylation of aryl iodide and bromide to access glycosyl aryl sulfones [J]. | ORGANIC & BIOMOLECULAR CHEMISTRY , 2025 . |
MLA | Wang, Linyitian et al. "Copper-promoted late-stage glycosylsulfonylation of aryl iodide and bromide to access glycosyl aryl sulfones" . | ORGANIC & BIOMOLECULAR CHEMISTRY (2025) . |
APA | Wang, Linyitian , Guo, Huize , Luo, Jiaxin , Zhen, Wenxu , Wang, Shiping , Xie, Zailai et al. Copper-promoted late-stage glycosylsulfonylation of aryl iodide and bromide to access glycosyl aryl sulfones . | ORGANIC & BIOMOLECULAR CHEMISTRY , 2025 . |
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Transition metal-based electrocatalysts are a promising alternative to noble metal catalysts for electrochemical upgrading of biomass-derived 5-hydroxymethylfurfural (HMF) into high-value 2,5-furandicarboxylic acid (FDCA). However, the rational design of efficient electrocatalysts with precisely tailored structure–activity correlations remains a critical challenge. Herein, we report a hierarchically structured self-supporting electrode (Vo-NiCo(OH)2-NF) synthesized through in situ electrochemical reconstruction of NiCo-Prussian blue analogue (NiCo-PBA) precursor, in which oxygen vacancy (Vo)-rich Co-doped Ni(OH)2 nanosheet arrays are vertically aligned on nickel foam (NF), creating an interconnected conductive network. When evaluated for the HMF oxidation reaction (HMFOR), Vo-NiCo(OH)2-NF exhibits exceptional electrochemical performance, achieving near-complete HMF conversion (99%), ultrahigh FDCA Faradaic efficiency (97.5%), and remarkable product yield (96.2%) at 1.45 V, outperforming conventional Co-doped Ni(OH)2 (NiCo(OH)2-NF) and pristine Ni(OH)2 (Ni(OH)2-NF) electrodes. By combining in situ spectroscopic characterization and theoretical calculations, we elucidate that the synergistic effects of Co-doping and oxygen vacancy engineering effectively modulate the electronic structure of Ni active centers, favor the formation of high-valent Ni3+ species, and optimize HMF adsorption, thereby improving the HMFOR performance. This work provides valuable mechanistic insights for catalyst design and may inspire the development of advanced transition metal-based electrodes for efficient biomass conversion systems. © 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences.
Keyword :
Coated wire electrodes Coated wire electrodes Electrolytic reduction Electrolytic reduction Nanosheets Nanosheets Reconstruction (structural) Reconstruction (structural) Structural analysis Structural analysis Structural dynamics Structural dynamics
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GB/T 7714 | Xie, Diexin , Chen, Jiabin , Hou, Jingxin et al. Rational design of oxygen vacancy-rich self-supporting NiCo(OH)2 electrode for efficient biomass upgrading [J]. | Journal of Energy Chemistry , 2025 , 108 : 558-566 . |
MLA | Xie, Diexin et al. "Rational design of oxygen vacancy-rich self-supporting NiCo(OH)2 electrode for efficient biomass upgrading" . | Journal of Energy Chemistry 108 (2025) : 558-566 . |
APA | Xie, Diexin , Chen, Jiabin , Hou, Jingxin , Yang, Fangfang , Feng, Runping , Cao, Changsheng et al. Rational design of oxygen vacancy-rich self-supporting NiCo(OH)2 electrode for efficient biomass upgrading . | Journal of Energy Chemistry , 2025 , 108 , 558-566 . |
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Carbon materials have stimulated tremendous interest in oxidative dehydrogenation (ODH) of alkane to olefin molecules at low temperature. Unfortunately, its further development has been seriously hindered due to the unsatisfactory catalytic performance. To tackle these challenges, nitrogen and phosphorus codoped hollow carbon prisms (NPC) are designed with controllable surface functional groups through supramolecular preassembly and substitution reaction from guanine and hexachlorotriphosphazene. The resultant catalysts can achieve both high catalytic activity (63 % conversion) and styrene selectivity (90 %) in ODH of ethylbenzene, outerperforming previous reported carbon-based catalysts. Structural characterizations, kinetics measurements and theoretical results unravel that nitrogen doping can promote nucleophilicity of -C--O, thus improving the catalytic activity. The phosphorus doping not only changes reaction rate-determining step from activation of O2 in N-doped carbon to activation of -C-H bond of EB in N,P-codoped carbon, but also inhibits the formation of electrophilic oxygen species, which enhances selectivity of styrene. The current work provides a facile strategy for preparation of functional NPC catalyst and physical-chemical insights on the structure-activity relationship of NPC catalysts, paving the way for further development of the highly efficient non-metallic catalytic systems.
Keyword :
Carbon prism Carbon prism Catalytic mechanism Catalytic mechanism Guanine Guanine Heteroatom doping Heteroatom doping Oxidative dehydrogenation Oxidative dehydrogenation
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GB/T 7714 | Zhang, Xuefei , Hu, Aoxue , Li, Shuchun et al. N, P codoped hollow carbon prisms for efficient oxidative dehydrogenation reaction with both enhanced activity and selectivity [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 486 . |
MLA | Zhang, Xuefei et al. "N, P codoped hollow carbon prisms for efficient oxidative dehydrogenation reaction with both enhanced activity and selectivity" . | CHEMICAL ENGINEERING JOURNAL 486 (2024) . |
APA | Zhang, Xuefei , Hu, Aoxue , Li, Shuchun , Feng, Ruiping , Huang, Shuping , Xie, Zailai . N, P codoped hollow carbon prisms for efficient oxidative dehydrogenation reaction with both enhanced activity and selectivity . | CHEMICAL ENGINEERING JOURNAL , 2024 , 486 . |
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Biomolecule self-assembly shows great potential in the preparation of ordered functional materials. Here, we prepare a gauzy NC material via water guiding guanine biomolecule self-assemble, which exhibits the better ethylbenzene conversion (similar to 50%), styrene selectivity (similar to 91%) and long-term stability (>40 h) in ODH of ethylbenzene to styrene than that of guanine solid self-assembly produced NC (38% conversion vs. 88% selectivity) sample. The study shows that water not only facilitates guanine biomolecule self-assembly to form more stable octamer structure but restrains vertical growth of guanine, and resultant NC-1000-12 h holds high density active sites and outstanding oxidation resistance, thus enhancing NC catalytic performance. Overall, current work provides a new understanding on preparation of highly efficient NC materials through supramolecular self-assembly strategy.
Keyword :
Guanine biomolecule Guanine biomolecule Nitrogen doping Nitrogen doping Oxidative dehydrogenation Oxidative dehydrogenation Self-assembly Self-assembly Water Water
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GB/T 7714 | Feng, Runping , Yin, Mengqi , Xie, Diexin et al. Guanine biomolecule derived nitrogen-doped carbon for efficient oxidative dehydrogenation performance [J]. | APPLIED CATALYSIS O: OPEN , 2024 , 193 . |
MLA | Feng, Runping et al. "Guanine biomolecule derived nitrogen-doped carbon for efficient oxidative dehydrogenation performance" . | APPLIED CATALYSIS O: OPEN 193 (2024) . |
APA | Feng, Runping , Yin, Mengqi , Xie, Diexin , Li, Shuchun , Zhang, Xuefei , Xie, Zailai . Guanine biomolecule derived nitrogen-doped carbon for efficient oxidative dehydrogenation performance . | APPLIED CATALYSIS O: OPEN , 2024 , 193 . |
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Developing novel electrocatalysts for achieving high selectivity and faradaic efficiency in the carbon dioxide reduction reaction (CO2RR) poses a major challenge. In this study, a catalyst featuring a nitrogen-doped carbon shell-coated Ni nanoparticle structure is designed for efficient carbon dioxide (CO2) electroreduction to carbon monoxide (CO). The optimal Ni@NC-1000 catalyst exhibits remarkable CO faradaic efficiency (FECO) values exceeding 90% across a broad potential range of -0.55 to -0.9 V (vs. RHE), and attains the maximum FECO of 95.6% at -0.75 V (vs. RHE) in 0.5 M NaHCO3. This catalyst exhibits sustained carbon dioxide electroreduction activity with negligible decay after continuous electrolysis for 20 h. More encouragingly, a substantial current density of 200.3 mA cm(-2) is achieved in a flow cell at -0.9 V (vs. RHE), reaching an industrial-level current density. In situ Fourier transform infrared spectroscopy and theoretical calculations demonstrate that its excellent catalytic performance is attributed to highly active pyrrolic nitrogen sites, promoting CO2 activation and significantly reducing the energy barrier for generating *COOH. To a considerable extent, this work presents an effective strategy for developing high-efficiency catalysts for electrochemical CO2 reduction across a wide potential window.
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GB/T 7714 | Peng, Ying , Chen, Shuo , Hu, Zhengli et al. Guanine-derived carbon nanosheet encapsulated Ni nanoparticles for efficient CO2 electroreduction [J]. | DALTON TRANSACTIONS , 2024 , 53 (23) : 9724-9731 . |
MLA | Peng, Ying et al. "Guanine-derived carbon nanosheet encapsulated Ni nanoparticles for efficient CO2 electroreduction" . | DALTON TRANSACTIONS 53 . 23 (2024) : 9724-9731 . |
APA | Peng, Ying , Chen, Shuo , Hu, Zhengli , Yin, Mengqi , Pei, Lishun , Wei, Qiaohua et al. Guanine-derived carbon nanosheet encapsulated Ni nanoparticles for efficient CO2 electroreduction . | DALTON TRANSACTIONS , 2024 , 53 (23) , 9724-9731 . |
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5-Hydroxymethylfurfural (HMF) is a widely used biomass platform chemical that plays a crucial role in bridging biomass and fossil resources. Electrocatalytic oxidation of HMF provides an efficient way to obtain high-value-added biomass-derived chemicals, among which the intermediate product 5-formyl-2-furan carboxylic acid (FFCA) has attracted considerable attention. However, the weak adsorption ability of monometallic nickel oxide (NiOx) to HMF in neutral electrolyte restricts its further development, resulting in low HMF conversion and FFCA yield. In this study, we successfully constructed a novel nickel oxide-platinum oxide hybrid catalyst supported on carbon felt (NiOx-PtOx/CF), which exhibits an optimized adsorption ability of HMF, leading to the outstanding FFCA yield up to 77 % in the neutral media. The high activity of the NiOx-PtOx/CF catalyst can be attributed to the redistribution of the electrons and the optimization of the electronic structure on the Ni active site due to the introduction of PtOx on NiOx nanosheets. This study offers valuable insights for the design of efficient multicomponent electrocatalysts for electrocatalytic biomass refinery systems. Highly efficient of HMF into FFCA on a NiOx-PtOx/carbon felt composite electrode is achieved at a potential of 1.78 VRHE with high value product of FFCA yield up to 77 %. The high activity of the NiOx-PtOx/CF catalyst can be attributed to the redistribution of the electrons and the optimization of the electronic structure on the Ni active site due to the introduction of PtOx on NiOx nanosheets. image
Keyword :
5-hydroxymethylfurfural 5-hydroxymethylfurfural bimetallic catalysts bimetallic catalysts electronic regulation electronic regulation Electrooxidation Electrooxidation formyl-2-furancarboxylic acid formyl-2-furancarboxylic acid
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GB/T 7714 | Wang, Di , Lu, Xingyu , Xu, Haiyan et al. Selective Synthesis of Formyl-2-Furancarboxylic Acid via Enhanced Adsorption of 5-Hydroxymethylfurfural on Composite Catalysts [J]. | CHEMCATCHEM , 2024 , 16 (18) . |
MLA | Wang, Di et al. "Selective Synthesis of Formyl-2-Furancarboxylic Acid via Enhanced Adsorption of 5-Hydroxymethylfurfural on Composite Catalysts" . | CHEMCATCHEM 16 . 18 (2024) . |
APA | Wang, Di , Lu, Xingyu , Xu, Haiyan , Dou, Jing , Zhang, Xuefei , Xie, Zailai et al. Selective Synthesis of Formyl-2-Furancarboxylic Acid via Enhanced Adsorption of 5-Hydroxymethylfurfural on Composite Catalysts . | CHEMCATCHEM , 2024 , 16 (18) . |
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Maximization the synergistic effect of each component in transition metal-carbon complexes is expected to improve the bifunctional oxygen electrocatalysis for rechargeable Zn-air batteries but is still challenging. Herein, nucleobase guanine is employed as a supramolecular precursor to generate the core (FeCo alloy)-shell (carbon) structure embedded in ultrathin graphene-like nitrogen-doped carbon nanosheets (FeCo@NCNSs) via a confinement pyrolysis strategy. Thanks to the generated core-shell structure and bimetallic synergistic effect, the as-prepared FeCo@NCNSs exhibits excellent electrochemical performance in both oxygen reduction reaction and oxygen evolution reaction. As a result, when served as the bifunctional air electrode for a practical Zn-air battery, FeCo@NCNSs exhibits a higher open-circuit voltage (1.553 V) and peak power density (197.30 mW cm-2), as well as the greatly improved long-term cyclic stability compared to the noble metal benchmarks. This work provides a promising approach to integrate various active sites for bifunctional oxygen electrocatalysis and inspires the exploration of simple but efficient electrocatalysts for energy storage and conversion.
Keyword :
Bifunctional oxygen electrocatalysis Bifunctional oxygen electrocatalysis Core-shell structure Core-shell structure FeCo alloy FeCo alloy Guanine Guanine Rechargeable Zn-air batteries Rechargeable Zn-air batteries
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GB/T 7714 | Lin, Xin , Cui, Longji , Ding, Xueda et al. Guanine-derived core-shell FeCo alloy confined in graphene-like N-doped carbon as efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries [J]. | JOURNAL OF ALLOYS AND COMPOUNDS , 2024 , 998 . |
MLA | Lin, Xin et al. "Guanine-derived core-shell FeCo alloy confined in graphene-like N-doped carbon as efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries" . | JOURNAL OF ALLOYS AND COMPOUNDS 998 (2024) . |
APA | Lin, Xin , Cui, Longji , Ding, Xueda , Chen, Yiquan , Wei, Qiaohua , Huang, Baobing et al. Guanine-derived core-shell FeCo alloy confined in graphene-like N-doped carbon as efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries . | JOURNAL OF ALLOYS AND COMPOUNDS , 2024 , 998 . |
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Borocarbonitride (BCN) catalysts, boasting multiple redox sites, have shown considerable potential in alkane oxidative dehydrogenation (ODH) to olefin molecules. However, their catalytic efficiency still lags behind that of leading commercial catalysts, primarily due to the limited reactivity of oxygen functional groups. In this study, a groundbreaking hybrid catalyst is developed, featuring BCN nanotubes (BCNNTs) encapsulated with manganese (Mn) clusters, crafted through a meticulous supramolecular self-assembly and postcalcination strategy. This novel catalyst demonstrates a remarkable enhancement in activity, achieving 30% conversion and approximate to 100% selectivity toward styrene in ethylbenzene ODH reactions. Notably, its performance surpasses both pure BCNNTs and those hosting Mn nanoparticles. Structural and kinetic analyses unveil a robust interaction between BCNNTs and the Mn component, substantially boosting the catalytic activity of BCNNTs. Furthermore, density functional theory (DFT) calculations elucidate that BCNNTs encapsulated with Mn clusters not only stabilize key intermediates (& horbar;B & horbar;O & horbar;O & horbar;B & horbar;) but also enhance the nucleophilicity of active sites through electron transfer from the Mn cluster to the BCNNTs. This electron transfer mechanism effectively lowers the energy barrier for & horbar;C & horbar;H cleavage, resulting in a 13% improvement in catalytic activity compared to pure BCNNTs. Manganese (Mn) cluster promoters enhance the catalytic activity of borocarbonitride in ethylbenzene oxidative dehydrogenation with approximate to 100% styrene selectivity, superior to these of unmodified and Mn particle-modified borocarbonitride materials, and the nature of activity improvement and reaction mechanism is revealed by combining with structural characterizations and density functional theory calculations. image
Keyword :
borocarbonitride nanotubes borocarbonitride nanotubes heterogeneous catalysis heterogeneous catalysis Mn modfication Mn modfication oxidative dehydrogenation oxidative dehydrogenation strong interaction strong interaction
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GB/T 7714 | Zhang, Xuefei , Dai, Xueya , Xie, Zailai et al. Borocarbonitride Catalyzed Ethylbenzene Oxidative Dehydrogenation: Activity Enhancement via Encapsulation of Mn Clusters inside the Tube [J]. | SMALL , 2024 , 20 (37) . |
MLA | Zhang, Xuefei et al. "Borocarbonitride Catalyzed Ethylbenzene Oxidative Dehydrogenation: Activity Enhancement via Encapsulation of Mn Clusters inside the Tube" . | SMALL 20 . 37 (2024) . |
APA | Zhang, Xuefei , Dai, Xueya , Xie, Zailai , Qi, Wei . Borocarbonitride Catalyzed Ethylbenzene Oxidative Dehydrogenation: Activity Enhancement via Encapsulation of Mn Clusters inside the Tube . | SMALL , 2024 , 20 (37) . |
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