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学者姓名：林伟
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Abstract ：
Carbon nitrides form a series of polymer semiconductors popular in photocatalysis. In the course of photoresponse, the separation of light-induced electron-hole pairs is one of the critical factors that affect the conversion rate from photoenergy to chemical substance. Exciton binding energy (Eb) is treated as a classical parameter to evaluate the barrier of exciton dissociation. In this work, we study the electronic and optical nature of two specific members of the carbon nitride family, polymeric carbon nitride (melon) and crystallized poly(triazine imide) (PTI/Li+Cl-) by employing the photoluminescence spectra and density functional theory (DFT) calculations based on the Wannier-Mott exciton module. The results of self-consistent GW computation were applied. The measurement of photoluminescence spectra, by which exciton binding energies are estimated, is likewise discussed. Generally, compared with the results calculated by GW-BSE, the DFT results based on the Wannier-Mott model are closer to the experimental values. From a materials perspective, on the other hand, the exciton binding energy of the melon is lower than that of PTI/Li+Cl-.
Keyword ：
carbon nitride carbon nitride DFT calculation DFT calculation exciton binding energy exciton binding energy photoluminescence spectra photoluminescence spectra
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| GB/T 7714 | Lin, Zhiyou , Cai, Xu , Lin, Wei . Investigation into the Exciton Binding Energy of Carbon Nitrides on Band Structure and Carrier Concentration through the Photoluminescence Effect [J]. | CATALYSTS , 2024 , 14 (4) . |
| MLA | Lin, Zhiyou 等. "Investigation into the Exciton Binding Energy of Carbon Nitrides on Band Structure and Carrier Concentration through the Photoluminescence Effect" . | CATALYSTS 14 . 4 (2024) . |
| APA | Lin, Zhiyou , Cai, Xu , Lin, Wei . Investigation into the Exciton Binding Energy of Carbon Nitrides on Band Structure and Carrier Concentration through the Photoluminescence Effect . | CATALYSTS , 2024 , 14 (4) . |
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Two novel vanadoborate compounds, [Cu(en)2]3[Li(H2O)]4[Li(H2O)3]2[V12B18O50(OH)10(H2O)]2 & sdot;33.5H2O (1) and (H2en)4[Li(H2O)]4[V12B18O55(OH)5(H2O)]& sdot;14H2O (2), were synthesized via hydrothermal synthesis under identical conditions except for temperature. Structural analysis revealed that although both contain [V12B18O60]n- cluster anion, the different countercations potentially lead to variations in the [V12B18O60]ncluster anion skeletons. In compound 1, the V4+/V5+ ratio was 10:2; while in compound 2 the ratio was 11:1. It is speculated that different countercations may influence the valence states of cluster anions. In this study, quantum chemical calculations revealed that the aromaticity and activity of the two compounds were different, and twodimensional correlation infrared spectroscopy (2D-COS-IR) under magnetic perturbation confirmed that distinct response peaks of functional group vibrations to the magnetic field due to the different V4+/V5+ ratios and aromaticity of the two compounds. An electrochemical analysis revealed that compound 2 exhibits higher electrocatalytic activity. The results of quantum chemical calculations are aligned not only with the changes in the 2D-COS-IR spectra but also with the conclusions obtained from experiments on electrochemical properties. Overall, this work proposes a novel strategy for interpreting the alteration of vanadoborate anionic skeleton due to the introduction of different countercations by combining 2D-COS-IR with quantum chemical calculations.
Keyword ：
Electrocatalyst Electrocatalyst Quantum chemical calculation Quantum chemical calculation spectroscopy spectroscopy Two-dimensional correlation infrared Two-dimensional correlation infrared Vanadoborate Vanadoborate
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| GB/T 7714 | Meng, Ming-Ze , Shi, Gui-Dong , Cheng, Ling-Ling et al. Two-dimensional correlation infrared spectroscopy study on vanadoborate anionic skeleton regulated by countercations [J]. | SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY , 2024 , 311 . |
| MLA | Meng, Ming-Ze et al. "Two-dimensional correlation infrared spectroscopy study on vanadoborate anionic skeleton regulated by countercations" . | SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY 311 (2024) . |
| APA | Meng, Ming-Ze , Shi, Gui-Dong , Cheng, Ling-Ling , Chen, Yi-Ping , Zhang, Yong-Fan , Lin, Wei . Two-dimensional correlation infrared spectroscopy study on vanadoborate anionic skeleton regulated by countercations . | SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY , 2024 , 311 . |
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Poly(triazine imide)Li+Cl- (PTI/Li+Cl-) as one of the most reported crystalline carbon nitrides has shown exciting potential for photocatalysis. However, understanding the role of Li+/Cl- in the photoexcited charge transfer in the time and space of PTI is a challenging problem. Here, we have investigated the nonradiative charge recombination of series ion intercalated PTI systems (PTI/Li+X-, where X = F, Cl, Br, and I) by performing the ab initio nonadiabatic molecular dynamics simulations. The results indicate that the intercalated anions in PTI/Li+Cl- and PTI/Li+Br- have the potential to trap holes, separate the electrons and holes, and prolong the nonradiative electron-hole recombination. In particular, similar to 70% of holes in PTI/Li+Cl- can transport among interlayers toward the {0001} planes, while most of the electrons are transferred to the {1010} planes, exhibiting different transport pathways and directions. Furthermore, PTI/Li+Cl- has an electron-hole recombination time as long as 136 ns, which explains its excellent optoelectronic properties. This work provides a theoretical baseline for the reported facet engineering improvement of crystalline carbon nitride for overall water splitting.
Keyword ：
charge carrierlifetime charge carrierlifetime crystalline carbon nitride crystalline carbon nitride lithium halide lithium halide recombination time recombination time spatial separation of electron and hole spatial separation of electron and hole
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| GB/T 7714 | Cai, Xu , Lin, Wei . Chloride Ion-Induced Spatial Separation and Long Recombination Time of Photogenerated Electrons and Holes in Crystalline Carbon Nitride [J]. | JACS AU , 2024 . |
| MLA | Cai, Xu et al. "Chloride Ion-Induced Spatial Separation and Long Recombination Time of Photogenerated Electrons and Holes in Crystalline Carbon Nitride" . | JACS AU (2024) . |
| APA | Cai, Xu , Lin, Wei . Chloride Ion-Induced Spatial Separation and Long Recombination Time of Photogenerated Electrons and Holes in Crystalline Carbon Nitride . | JACS AU , 2024 . |
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H2S selective catalytic oxidation via photocatalysis is a low-cost and efficient approach. Herein, we modeled a (CoP)4 cluster loaded melon-based carbon nitride to represent experimental cobalt phosphate cocatalyst adsorption on polymeric carbon nitride for revealing the mechanism of H2S selective catalytic oxidation to SO2 via the density functional theory (DFT) calculations. Due to the hydrogen bond effect, the calculated results show that H2S selective oxidation prefers to occur through the quasi Mars-van Krevelen (quasi-MvK) mechanism rather than Langmuir-Hinshelwood (LH) mechanism according to the thermodynamic perspective, in which quasi-MvK mechanism exhibits a favorable limiting potential of 0.26 V. Overall, this work offers a basic understanding for microscopic mechanism of H2S catalytic oxidation.
Keyword ：
Carbon nitride Carbon nitride CoP cluster CoP cluster DFT calculations DFT calculations H 2 S selective oxidation H 2 S selective oxidation
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| GB/T 7714 | Xu, Hongli , Yang, Wanxiang , Yang, Can et al. Unraveling the H2S selective oxidation in cobalt phosphate cluster loaded polymeric carbon nitride [J]. | SURFACES AND INTERFACES , 2024 , 46 . |
| MLA | Xu, Hongli et al. "Unraveling the H2S selective oxidation in cobalt phosphate cluster loaded polymeric carbon nitride" . | SURFACES AND INTERFACES 46 (2024) . |
| APA | Xu, Hongli , Yang, Wanxiang , Yang, Can , Lin, Wei . Unraveling the H2S selective oxidation in cobalt phosphate cluster loaded polymeric carbon nitride . | SURFACES AND INTERFACES , 2024 , 46 . |
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As typical representatives of group III chalcogenides, InSe, alpha -In2Se3, and beta ' -In2Se3 have drawn considerable interest in the domain of photoelectrochemistry. However, the microscopic mechanisms of carrier dynamics in these systems remain largely unexplored. In this work, we first reveal that hot electrons in the three systems have different cooling rate stages and long-lived hot electrons, through the utilization of density functional theory calculations and nonadiabatic molecular dynamics simulations. Furthermore, the ferroelectric polarization of alpha -In2Se3 weakens the nonadiabatic coupling of the nonradioactive recombination, successfully competing with the narrow bandgap and slow dephasing process, and achieving both high optical absorption efficiency and long carrier lifetime. In addition, we demonstrate that the ferroelectric polarization of alpha -In2Se3 not only enables the formation of the double type-II band alignment in the InSe/alpha -In2Se3/InSe heterostructure, with the top and bottom InSe sublayers acting as acceptors and donors, respectively, but also eliminates the hindrance of the built-in electric field at the interface, facilitating an ultrafast interlayer carrier transfer in the heterojunction. This work establishes an atomic mechanism of carrier dynamics in InSe, alpha -In2Se3, and beta ' -In2Se3 and the regulatory role of the ferroelectric polarization on the charge carrier dynamics, providing a guideline for the design of photoelectronic materials.
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| GB/T 7714 | Lau, Guanghua , Li, Yi , Zhang, Yongfan et al. Reveal long-lived hot electrons in 2D indium selenide and ferroelectric-regulated carrier dynamics of InSe/α-In2Se3/InSe heterostructure [J]. | JOURNAL OF CHEMICAL PHYSICS , 2024 , 160 (12) . |
| MLA | Lau, Guanghua et al. "Reveal long-lived hot electrons in 2D indium selenide and ferroelectric-regulated carrier dynamics of InSe/α-In2Se3/InSe heterostructure" . | JOURNAL OF CHEMICAL PHYSICS 160 . 12 (2024) . |
| APA | Lau, Guanghua , Li, Yi , Zhang, Yongfan , Lin, Wei . Reveal long-lived hot electrons in 2D indium selenide and ferroelectric-regulated carrier dynamics of InSe/α-In2Se3/InSe heterostructure . | JOURNAL OF CHEMICAL PHYSICS , 2024 , 160 (12) . |
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The selective conversion of ethane (C2H6) to ethylene (C2H4) under mild conditions is highly wanted, yet very challenging. Herein, it is demonstrated that a Pt/WO3-x catalyst, constructed by supporting ultrafine Pt nanoparticles on the surface of oxygen-deficient tungsten oxide (WO3-x) nanoplates, is efficient and reusable for photocatalytic C2H6 dehydrogenation to produce C2H4 with high selectivity. Specifically, under pure light irradiation, the optimized Pt/WO3-x photocatalyst exhibits C2H4 and H2 yield rates of 291.8 and 373.4 mu mol g-1 h-1, respectively, coupled with a small formation of CO (85.2 mu mol g-1 h-1) and CH4 (19.0 mu mol g-1 h-1), corresponding to a high C2H4 selectivity of 84.9%. Experimental and theoretical studies reveal that the vacancy-rich WO3-x catalyst enables broad optical harvesting to generate charge carriers by light for working the redox reactions. Meanwhile, the Pt cocatalyst reinforces adsorption of C2H6, desorption of key reaction species, and separation and migration of light-induced charges to promote the dehydrogenation reaction with high productivity and selectivity. In situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory calculation expose the key intermediates formed on the Pt/WO3-x catalyst during the reaction, which permits the construction of the possible C2H6 dehydrogenation mechanism. The Pt/WO3-x photocatalyst consisted of ultrafine Pt nanoparticles supported on the surface of oxygen-defective tungsten oxide nanoplates manifests high activity and fine reusability for selective ethylene formation from ethane dehydrogenation by simulated sunlight under mild conditions. image
Keyword ：
ethylene production ethylene production lattice oxygen lattice oxygen oxygen vacancy oxygen vacancy photocatalysis photocatalysis tungsten oxide tungsten oxide
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| GB/T 7714 | Liu, Yue , Xue, Weichao , Liu, Xiaoqing et al. Ultrafine Pt Nanoparticles on Defective Tungsten Oxide for Photocatalytic Ethylene Synthesis [J]. | SMALL , 2024 . |
| MLA | Liu, Yue et al. "Ultrafine Pt Nanoparticles on Defective Tungsten Oxide for Photocatalytic Ethylene Synthesis" . | SMALL (2024) . |
| APA | Liu, Yue , Xue, Weichao , Liu, Xiaoqing , Wei, Fen , Lin, Xiahui , Lu, Xue Feng et al. Ultrafine Pt Nanoparticles on Defective Tungsten Oxide for Photocatalytic Ethylene Synthesis . | SMALL , 2024 . |
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Aerobic photocatalytic oxidation is considered as an efficient and green method to remedy low-concentration H2S pollutants associated with the energy and chemical industries. However, the fabrication of a sulfur-resistant catalyst with good performance is a great challenge because of the poisoning effect of H2S and the difficulty in oxygen (O-2) activation. Herein, a photocatalytic hybrid material composed of chemically stable cobalt phosphide (CoP) and structural base-enriched carbon nitride (CN) was developed for the efficient oxidation of H2S, which could achieve 95% H2S conversion, and its service time could last more than 35 h with over 80% H2S conversion. Reflecting from the characterizations and theoretical simulations, the enhanced H2S conversion was on account that CoP could stimulate the electrons shuttling from the photocatalytic system towards the gaseous O-2, facilitating the production of critical superoxide radical via the O-2 reduction process and accelerating the surface H2S oxidation process. This work provides new insights into the design of a sustainable photocatalytic oxidation system for the treatment of chemically active contaminants through constructing stable interfacial electron transfer channels for prominent O-2 activation.
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| GB/T 7714 | Wang, Jiali , Chen, Biqi , Zeng, Fanghua et al. Boosting oxygen activation by CoP/carbon nitride photocatalyst in low-concentration H2S oxidation [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2024 . |
| MLA | Wang, Jiali et al. "Boosting oxygen activation by CoP/carbon nitride photocatalyst in low-concentration H2S oxidation" . | JOURNAL OF MATERIALS CHEMISTRY A (2024) . |
| APA | Wang, Jiali , Chen, Biqi , Zeng, Fanghua , Lu, Xue Feng , Hou, Yidong , Lin, Wei et al. Boosting oxygen activation by CoP/carbon nitride photocatalyst in low-concentration H2S oxidation . | JOURNAL OF MATERIALS CHEMISTRY A , 2024 . |
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The integration of heterogeneous photocatalysts with nickel catalysis is garnering considerable interest for their capacity to enable distinct metal-photoredox processes for organic synthesis. However, the challenge about robustness and recyclability of the photocatalyst persists. Herein, a crystalline carbon nitride (MCN-B) photocatalyst with intentionally introduced defects and a dedicated designed active site has been presented. Results reveal by incorporating the deprotonated cyano-group (N--CN) sites, this host material could provide stable binding sites for Ni (II) ions through the Hard-Soft Acid-Base (HSAB) effect, thereby facilitating charge transmission between semiconductor and metal centers. Consequently, the integrated carbon nitride nickel (Ni/MCNB) heterogeneous photocatalyst demonstrates high effectiveness in diverse photocatalytic C-N coupling reactions (21 examples, up to 93% yield) under conditions free from organic ligands and additives, which shows competent performance to the homogeneous catalysts. Moreover, the Ni/MCN-B catalyst demonstrates remarkable recyclability, maintaining its photoredox efficiency after 10 cycles with minimal loss of activity and a diminished metal leaching rate, which signifies a substantial advancement in the field of photocatalytic system design.
Keyword ：
Carbon nitride Carbon nitride Cross-coupling Cross-coupling Crystalline polymer Crystalline polymer Photocatalysis Photocatalysis
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| GB/T 7714 | Zhang, Huali , Chen, Xiaoxiao , Cheng, Jiajia et al. Heterogeneous metallaphotocatalytic Cross-Coupling reactions by a carbon Nitride-Nickel catalyst [J]. | JOURNAL OF CATALYSIS , 2024 , 433 . |
| MLA | Zhang, Huali et al. "Heterogeneous metallaphotocatalytic Cross-Coupling reactions by a carbon Nitride-Nickel catalyst" . | JOURNAL OF CATALYSIS 433 (2024) . |
| APA | Zhang, Huali , Chen, Xiaoxiao , Cheng, Jiajia , Yang, Xintuo , Lin, Wei , Hou, Yidong et al. Heterogeneous metallaphotocatalytic Cross-Coupling reactions by a carbon Nitride-Nickel catalyst . | JOURNAL OF CATALYSIS , 2024 , 433 . |
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Highly crystalline carbon nitride polymers have shown great opportunities in overall water photosplitting; however, their mission in light-driven CO2 conversion remains to be explored. In this work, crystalline carbon nitride (CCN) nanosheets of poly triazine imide (PTI) embedded with melon domains are fabricated by KCl/LiCl-mediated polycondensation of dicyandiamide, the surface of which is subsequently deposited with ultrafine WO3 nanoparticles to construct the CCN/WO3 heterostructure with a S-scheme interface. Systematic characterizations have been conducted to reveal the compositions and structures of the S-scheme CCN/WO3 hybrid, featuring strengthened optical capture, enhanced CO2 adsorption and activation, attractive textural properties, as well as spatial separation and directed movement of light-triggered charge carriers. Under mild conditions, the CCN/WO3 catalyst with optimized composition displays a high photocatalytic activity for reducing CO2 to CO in a rate of 23.0 mu mol/hr ( i.e., 2300 mu mol/(hr center dot g)), which is about 7-fold that of pristine CCN, along with a high CO selectivity of 90.6% against H2 formation. Moreover, it also manifests high stability and fine reusability for the CO2 conversion reaction. The CO2 adsorption and conversion processes on the catalyst are monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), identifying the crucial intermediates of CO2 *-, COOH* and CO*, which integrated with the results of performance evaluation proposes the possible CO2 reduction mechanism. (c) 2023 The Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences. Published by Elsevier B.V.
Keyword ：
CO 2 reduction CO 2 reduction Crystalline carbon nitride Crystalline carbon nitride Photocatalysis Photocatalysis S-scheme S-scheme WO3 WO3
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| GB/T 7714 | Chen, Gongjie , Zhou, Ziruo , Li, Bifang et al. S-scheme heterojunction of crystalline carbon nitride nanosheets and ultrafine WO3 nanoparticles for photocatalytic CO2 reduction [J]. | JOURNAL OF ENVIRONMENTAL SCIENCES , 2024 , 140 : 103-112 . |
| MLA | Chen, Gongjie et al. "S-scheme heterojunction of crystalline carbon nitride nanosheets and ultrafine WO3 nanoparticles for photocatalytic CO2 reduction" . | JOURNAL OF ENVIRONMENTAL SCIENCES 140 (2024) : 103-112 . |
| APA | Chen, Gongjie , Zhou, Ziruo , Li, Bifang , Lin, Xiahui , Yang, Can , Fang, Yuanxing et al. S-scheme heterojunction of crystalline carbon nitride nanosheets and ultrafine WO3 nanoparticles for photocatalytic CO2 reduction . | JOURNAL OF ENVIRONMENTAL SCIENCES , 2024 , 140 , 103-112 . |
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Dehydroepiandrosterone (DHEA) is an important neurosteroid hormone to keep human hormonal balance and reproductive health. However, DHEA was always produced with impurities either by chemical or biological method and required high-cost purification before the medical use. To address this issue, a novel chemo-enzymatic process was proposed and implemented to produce DHEA. An acetoxylated derivate of 4-androstene-3,17-dione (4-AD) was generated by chemical reaction and converted into DHEA by an enzyme cascade reaction combining a hydrolysis reaction with a reduction reaction. The hydrolysis reaction was catalyzed by a com-mercial esterase Z03 while the reduction reaction was catalyzed by E. coli cells co-expressing a 3 beta-hydroxysteroid dehydrogenase SfSDR and a glucose dehydrogenase BtGDH. After the condition optimization, DHEA was syn-thesized at a 100 mL scale under 100 mM of substrate loading and purified as white powder with the highest space-time yield (4.80 g/L/h) and purity (99 %) in the biosynthesis of DHEA. The successful attempt in this study provides a new approach for green synthesis of highly purified DHEA in the pharmaceutical industry.
Keyword ：
3?-hydroxysteroid dehydrogenase 3?-hydroxysteroid dehydrogenase Chemoenzymatic process Chemoenzymatic process Dehydroepiandrosterone Dehydroepiandrosterone Enzyme cascade Enzyme cascade Hydrolysis Hydrolysis
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| GB/T 7714 | Su, Bing-Mei , Shi, Yi-Bing , Lin, Wei et al. A chemoenzymatic process for preparation of highly purified dehydroepiandrosterone in high space-time yield [J]. | BIOORGANIC CHEMISTRY , 2023 , 133 . |
| MLA | Su, Bing-Mei et al. "A chemoenzymatic process for preparation of highly purified dehydroepiandrosterone in high space-time yield" . | BIOORGANIC CHEMISTRY 133 (2023) . |
| APA | Su, Bing-Mei , Shi, Yi-Bing , Lin, Wei , Xu, Lian , Xu, Xin-Qi , Lin, Juan . A chemoenzymatic process for preparation of highly purified dehydroepiandrosterone in high space-time yield . | BIOORGANIC CHEMISTRY , 2023 , 133 . |
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