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学者姓名：林伟
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Abstract ：
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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Creating useful chemicals or fuels from CO2 is one of the most promising ways to reach carbon neutral. In this work, through the formation of Lewis acid sites, a string of boron-atom-coordinated Ru single-atom catalysts (SACs), namely RuBxN4-x@TiN (x=0–4), were constructed, and their CO2 reduction reaction (CO2RR) was systematically studied. The results show that o-RuB2N2@TiN, p-RuB2N2@TiN, and RuB3N1@TiN are able to efficiently inhibit the competitive hydrogen evolution reaction (HER) and activate CO2, with a potential-determining step lower than 0.7 eV and high selectivity for CH4 generation. This work shows that the synergistic effect of B and Ru atoms are able to effectively improve the catalytic activity, which is expected to offer a possible tactic for the sensible creation of effective CO2RR catalysts. © 2024
Keyword ：
CO2 reduction CO2 reduction Coordination-tuned Coordination-tuned Density functional theory Density functional theory Lewis acid sites Lewis acid sites TiN TiN
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| GB/T 7714 | Pan, J. , Kong, Y. , Li, Y. et al. Coordination-tuned Ru single-atom catalyst for efficient catalysis of CO2 to CH4 on RuBxN4-x@TiN (x=0–4) [J]. | Journal of CO2 Utilization , 2024 , 84 . |
| MLA | Pan, J. et al. "Coordination-tuned Ru single-atom catalyst for efficient catalysis of CO2 to CH4 on RuBxN4-x@TiN (x=0–4)" . | Journal of CO2 Utilization 84 (2024) . |
| APA | Pan, J. , Kong, Y. , Li, Y. , Zhang, Y. , Lin, W. . Coordination-tuned Ru single-atom catalyst for efficient catalysis of CO2 to CH4 on RuBxN4-x@TiN (x=0–4) . | Journal of CO2 Utilization , 2024 , 84 . |
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Amorphous Ga2O3 thin films were deposited on SiO2 and sapphire substrates by pulsed magnetron sputtering (PSD) at room temperature, respectively. Corresponding amorphous Ga2O3 thin film photodetectors were prepared. The oxygen vacancies and defects of the interface between films and substrates were found to determine the discrepancy by comparing the performance between these two photodetectors. Amorphous Ga2O3 photodetectors on SiO2 had highly performances with a responsivity of 417 A/W, detectivity of 7.84 x 1012 Jones, and external quantum efficiency of 2.01 x 105 %.
Keyword ：
Amorphous Amorphous Photodetectors Photodetectors
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| GB/T 7714 | Peng, Kai , Xue, DiFei , Lin, Wei et al. Amorphous Ga2O3-based solar-blind photodetectors on crystalline and amorphous substrates: A comparative study [J]. | MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING , 2024 , 179 . |
| MLA | Peng, Kai et al. "Amorphous Ga2O3-based solar-blind photodetectors on crystalline and amorphous substrates: A comparative study" . | MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING 179 (2024) . |
| APA | Peng, Kai , Xue, DiFei , Lin, Wei , Lv, PeiWen . Amorphous Ga2O3-based solar-blind photodetectors on crystalline and amorphous substrates: A comparative study . | MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING , 2024 , 179 . |
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Cadmium sulfide (CdS) exhibits remarkable light absorption capabilities and is widely employed in photocatalytic reduction of CO2. Nevertheless, the crystal facet effects on the micro-scale mechanisms governing CO2 conversion on CdS remain elusive. This study theoretically investigates the electronic properties of hexagonal-phase (101), (001), and cubic-phase (111) CdS surfaces modified with diethylenetriamine (DETA). From a microscopic viewpoint, it elucidates the unique bonding characteristics of CO2 on different exposed facets of DETA/CdS and the formation mechanisms leading to products such as CO, HCOOH, CH2O, CH3OH, and CH4. Our findings reveal that the DETA/CdS(101) surface is the most stable, effectively adsorbing hydrogen and CO2 at varied Cd sites with a high selectivity towards CO production, thereby showing promise for syngas generation, albeit with potential yields of formic acid and methane. Conversely, DETA/CdS(001) and (111) primarily facilitate the reduction of CO2 to CH4. These discoveries offer theoretical insights into photochemical experiments involving CO2 reduction on CdS, shedding light on the influence of crystal facets on reaction pathways.
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| GB/T 7714 | Guo, Meiyan , Yang, Wanxiang , Li, Yi et al. Mechanistic study of DETA-modified CdS for carbon dioxide reduction [J]. | CATALYSIS SCIENCE & TECHNOLOGY , 2024 , 14 (24) : 7172-7181 . |
| MLA | Guo, Meiyan et al. "Mechanistic study of DETA-modified CdS for carbon dioxide reduction" . | CATALYSIS SCIENCE & TECHNOLOGY 14 . 24 (2024) : 7172-7181 . |
| APA | Guo, Meiyan , Yang, Wanxiang , Li, Yi , Zhang, Yongfan , Lin, Wei . Mechanistic study of DETA-modified CdS for carbon dioxide reduction . | CATALYSIS SCIENCE & TECHNOLOGY , 2024 , 14 (24) , 7172-7181 . |
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The CO reduction reaction (CORR) for the production of high-value-added multi-carbon (C2+) products is currently being actively investigated, where searching for high-efficiency catalysts with moderate CO intermediate binding strength and low kinetic barrier for C-C coupling poses a significant challenge. In this study, we employed density functional theory computations to design four synergistic coupling dual sites catalysts for CORR to C-2 products, namely, TM-P@melon, by co-doping transition metals (TM = Mn, Fe, Co, and Ni) and phosphorus (P) into the polymeric carbon nitride (i.e., melon-CN). Mn-P@melon and Ni-P@melon exhibit higher selectivity toward C2H5OH and C2H6, respectively, with limiting potentials (C-C coupling kinetic energy barriers) of -0.43 V (0.52 eV) and -0.17 V (0.26 eV), respectively. The introduction of TM and P atoms not only narrows the band gap of melon-CN but also favors the coupling of CO and *CHO, providing an active site for C-C coupling, thus facilitating the catalytic reaction. Our work provides rational insights for the design of stable, low-cost, and efficient CORR dual sites catalysts that facilitate the sustainable production of high-value C-2 chemicals and fuels.
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| GB/T 7714 | Ji, Shuang , Lin, Wei . TM and P dual sites on polymeric carbon nitride enable highly selective CO reduction to C2 products with low potentials: A theoretical perspective [J]. | JOURNAL OF CHEMICAL PHYSICS , 2024 , 161 (17) . |
| MLA | Ji, Shuang et al. "TM and P dual sites on polymeric carbon nitride enable highly selective CO reduction to C2 products with low potentials: A theoretical perspective" . | JOURNAL OF CHEMICAL PHYSICS 161 . 17 (2024) . |
| APA | Ji, Shuang , Lin, Wei . TM and P dual sites on polymeric carbon nitride enable highly selective CO reduction to C2 products with low potentials: A theoretical perspective . | JOURNAL OF CHEMICAL PHYSICS , 2024 , 161 (17) . |
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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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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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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 et al. "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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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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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 , 20 (36) . |
| MLA | Liu, Yue et al. "Ultrafine Pt Nanoparticles on Defective Tungsten Oxide for Photocatalytic Ethylene Synthesis" . | SMALL 20 . 36 (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 , 20 (36) . |
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