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学者姓名：戴文新
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Abstract ：
CO2 conversion with pure H2O into CH3OH and O-2 driven by solar energy can supply fuels and life-essential substances for extraterrestrial exploration. However, the effective production of CH3OH is significantly challenging. Here we report an organozinc complex/MoS2 heterostructure linked by well-defined zinc-sulfur covalent bonds derived by the structural deformation and intensive coupling of dx 2 - y2(Zn)-p(S) orbitals at the interface, resulting in distinctive charge transfer behaviors and excellent redox capabilities as revealed by experimental characterizations and firstprinciple calculations. The synthesis strategy is further generalized to more organometallic compounds, achieving various heterostructures for CO2 photoreduction. The optimal catalyst delivers a promising CH3OH yield of 2.57 mmol gcat-1 h(-1) and selectivity of more than 99.5%. The reverse water gas shift mechanism is identified for methanol formation. Meanwhile, energy-unfavorable adsorption of methanol on MoS2, where the photogenerated holes accumulate, ensures the selective oxidation of water over methanol.
Keyword ：
CO2 photoreduction CO2 photoreduction extraterrestrial synthesis extraterrestrial synthesis methanol methanol strong metal-supportinteractions strong metal-supportinteractions two-dimensional heterostructures two-dimensional heterostructures
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| GB/T 7714 | Cheng, Ming , Cao, Ning , Wang, Zhi et al. Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O [J]. | ACS NANO , 2024 , 18 (15) : 10582-10595 . |
| MLA | Cheng, Ming et al. "Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O" . | ACS NANO 18 . 15 (2024) : 10582-10595 . |
| APA | Cheng, Ming , Cao, Ning , Wang, Zhi , Wang, Ke , Pu, Tiancheng , Li, Yukun et al. Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O . | ACS NANO , 2024 , 18 (15) , 10582-10595 . |
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The construction of photothermal catalysts to provide advanced oxidation ability and stability is a great challenge for eliminating volatile organic compounds (VOCs) during the photothermal catalytic process. Herein, a bimetallic modification method was proposed to synthesize Pd/Fe-TiO2. Under ultraviolet-visible (UV-Vis) light irradiation with the intensity of 610 mW/cm(2), the optimal 0.7 wt% Pd/0.4 wt% Fe-TiO2 catalyst of which surface was detected at the temperature of 165 C can achieve a toluene conversion of 94 % and a CO2 yield of 87 %, respectively. Based on the results of in-situ DRIFTS, quasi-situ EPR, XPS, and O-2-TPD tests, it was found that two distinct types of Pd and Fe active sites not only generated reactive oxygen species (ROS) but also adsorbed toluene and intermediate species, which promoted the degradation of toluene. It is proposed that there be an electron transfer behavior between Fe and Pd nanoparticles, resulting in a synergistic interaction of the two metals. This study shows that creating bimetallic modification catalysts is an efficient method for eliminating VOCs through photothermal catalysis.
Keyword ：
Bimetallic modification Bimetallic modification Oxidative degradation Oxidative degradation Photothermal catalysis Photothermal catalysis ROS ROS Toluene Toluene
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| GB/T 7714 | Fan, Shipeng , Luo, Songyu , Wang, Yun et al. TiO2-based Pd/Fe bimetallic modification for the efficient photothermal catalytic degradation of toluene: The synergistic effect of •O2- and •OH species [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 336 . |
| MLA | Fan, Shipeng et al. "TiO2-based Pd/Fe bimetallic modification for the efficient photothermal catalytic degradation of toluene: The synergistic effect of •O2- and •OH species" . | SEPARATION AND PURIFICATION TECHNOLOGY 336 (2024) . |
| APA | Fan, Shipeng , Luo, Songyu , Wang, Yun , Yue, Xuanyu , Zheng, Duojia , Zhang, Zizhong et al. TiO2-based Pd/Fe bimetallic modification for the efficient photothermal catalytic degradation of toluene: The synergistic effect of •O2- and •OH species . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 336 . |
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Pollution in water environments hinders both social progress and economic development. Wastewater treatment and the sustainable use of water resources are important factors in solving this problem. In a previous study, the authors proposed a process that used photocatalytic film as a back-end treatment in a composite iron-carbon constructed wetland (WIC&PF) to restore a mildly eutrophic water body. This method has strong reoxygenation effects, and can efficiently remove pollutants; these are qualities that have not been mentioned in previous studies regarding constructed wetlands. In this study, the authors further investigated the effectiveness of this process by using a photocatalytic film as a front-end treatment for a composite iron-carbon constructed wetland (PF&WIC) to restore a mildly eutrophic water body. The results showed NH4+-N, TN, TP, COD, and chlorophyll a removal rates using PF&WIC of 79.1 +/- 6.6%, 76.8 +/- 6.5%, 77.0 +/- 5.4%, 77.3 +/- 7.2%, and 91.7 +/- 5.6%, respectively. The DO concentration of the water body increased compared with that of the effluent. The bacterial species and their abundance in the lake water also changed significantly, and photosynthetic autotrophic bacteria (Cyanobium PCC-6307) became the most dominant bacteria, and this played an important role in reoxygenating the water body. In comparing these results to those of our previous study, the removal of pollutants with PF&WIC was close to that with WIC&PF, but the reoxygenation effect of PF&WIC on the water body was significantly worse than that of WIC & PF; thus, WIC&PF is the more reasonable choice for treating eutrophic water bodies.
Keyword ：
constructed wetland constructed wetland photoautotrophic bacteria photoautotrophic bacteria photocatalytic film photocatalytic film reoxygenation reoxygenation sustainable utilization sustainable utilization water pollution water pollution
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| GB/T 7714 | Chen, Shihao , Ye, Ming , Chen, Nuo et al. Study of a New Photocatalytic Film Process Combined with a Constructed Wetland and an Analysis of Reoxygenation Pathways in a Water Body [J]. | SUSTAINABILITY , 2024 , 16 (8) . |
| MLA | Chen, Shihao et al. "Study of a New Photocatalytic Film Process Combined with a Constructed Wetland and an Analysis of Reoxygenation Pathways in a Water Body" . | SUSTAINABILITY 16 . 8 (2024) . |
| APA | Chen, Shihao , Ye, Ming , Chen, Nuo , Pan, Wenbin , Dai, Wenxin . Study of a New Photocatalytic Film Process Combined with a Constructed Wetland and an Analysis of Reoxygenation Pathways in a Water Body . | SUSTAINABILITY , 2024 , 16 (8) . |
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Photocatalytic hydrogen production from formic acid (FA) is a daunting challenge, yet an essential task forthe development of hydrogen energy. In this study, a p-NiO/n-TiO2 heterojunction incorporating 7-nm metallic Ni was fabricated, which demonstrated a remarkable localized surface plasmon resonance (LSPR) effect. Notably, 5 wt% Ni/TiO2 exhibited 1271 -fold higher photocatalytic activity (2416 mu mol center dot g- 1 center dot h-1) than TiO2 alone under light radiation at room temperature. The experimental investigations revealed the excitation of distinct components via irradiation by different light sources. Visible light -driven hydrogen production was predominantly influenced by the LSPR-induced hot electrons and holes effects of Ni. Further, FA molecules simultaneously lost and accepted electrons at the Ni0-Ti3+ and Ni0-O2- sites, respectively, generating a bidirectional electron transfer behavior with "valley -shaped" gas -sensitive responses, which was crucial to boost the activity. Moreover, the photocatalytic activity was mainly attributed to the heterojunction and defects structure under UV light irradiation, and Ti3+, VOs, and O2- as adsorption sites for FA. Thus, the synergistic interplay among different light sources could effectively boost the photocatalytic hydrogen production performance. Significantly, this research reveals that the LSPR effect of metallic Ni can effectively regulate electron transfer behavior and enhance visible light -driven photocatalytic activity.
Keyword ：
Adsorption behavior Adsorption behavior Electron transfer Electron transfer formic acid formic acid Localized surface plasmon resonance (LSPR) Localized surface plasmon resonance (LSPR) Metallic Ni Metallic Ni Photocatalysis hydrogen production from Photocatalysis hydrogen production from
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| GB/T 7714 | Wang, Zhongming , Huang, Xiaoqian , Jia, Yong et al. Localized surface plasmon resonance-induced bidirectional electron transfer of formic acid adsorption for boosting photocatalytic hydrogen production on Ni/TiO2 [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 482 . |
| MLA | Wang, Zhongming et al. "Localized surface plasmon resonance-induced bidirectional electron transfer of formic acid adsorption for boosting photocatalytic hydrogen production on Ni/TiO2" . | CHEMICAL ENGINEERING JOURNAL 482 (2024) . |
| APA | Wang, Zhongming , Huang, Xiaoqian , Jia, Yong , Guo, Lina , Wang, Hong , Dai, Wenxin . Localized surface plasmon resonance-induced bidirectional electron transfer of formic acid adsorption for boosting photocatalytic hydrogen production on Ni/TiO2 . | CHEMICAL ENGINEERING JOURNAL , 2024 , 482 . |
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Halogenated methane serves as a universal platform molecule for building high-value chemicals. Utilizing sodium chloride solution for photocatalytic methane chlorination presents an environmentally friendly method for methane conversion. However, competing reactions in gas-solid-liquid systems leads to low efficiency and selectivity in photocatalytic methane chlorination. Here, an in situ method is employed to fabricate a hydrophobic layer of TaOx species on the surface of NaTaO3. Through in-situ XPS and XANES spectra analysis, it is determined that TaOx is a coordination unsaturated species. The TaOx species transforms the surface properties from the inherent hydrophilicity of NaTaO3 to the hydrophobicity of TaOx/NaTaO3, which enhances the accessibility of CH4 for adsorption and activation, and thus promotes the methane chlorination reaction within the gas-liquid-solid three-phase system. The optimized TaOx/NaTaO3 photocatalyst has a good durability for multiple cycles of methane chlorination reactions, yielding CH3Cl at a rate of 233 mu mol g(-1) h(-1) with a selectivity of 83%. In contrast, pure NaTaO3 exhibits almost no activity toward CH3Cl formation, instead catalyzing the over-oxidation of CH4 into CO2. Notably, the activity of the optimized TaOx/NaTaO3 photocatalyst surpasses that of reported noble metal photocatalysts. This research offers an effective strategy for enhancing the selectivity of photocatalytic methane chlorination using inorganic chlorine ions.
Keyword ：
hydrophobicity hydrophobicity methane chlorination methane chlorination photocatalysis photocatalysis TaOx TaOx ultrathin layer ultrathin layer
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| GB/T 7714 | Li, Dongmiao , Lin, Min , Zhang, Jiangjie et al. Hydrophobic TaOx Species Overlayer Tuning Light-Driven Methane Chlorination with Inorganic Chlorine [J]. | SMALL , 2024 , 20 (38) . |
| MLA | Li, Dongmiao et al. "Hydrophobic TaOx Species Overlayer Tuning Light-Driven Methane Chlorination with Inorganic Chlorine" . | SMALL 20 . 38 (2024) . |
| APA | Li, Dongmiao , Lin, Min , Zhang, Jiangjie , Qiu, Chengwei , Chen, Hui , Xiao, Zhen et al. Hydrophobic TaOx Species Overlayer Tuning Light-Driven Methane Chlorination with Inorganic Chlorine . | SMALL , 2024 , 20 (38) . |
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Constructing strong interfacial electric fields to enhance the surface charge transport kinetics is an effective strategy for promoting CO2 conversion. Herein, we present the fabrication of CdS-Bi2MoO6 Z-scheme heterojunctions with a robust internal electric field (IEF) using an in situ growth technique, establishing chemical bonding between the components. The IEF at the interface can offer an impetus for the segregation and transportation of photogenerated carriers, while the Cd-O chemical bonding mode acts as a rapid conduit for these carriers, thereby reducing the charge transfer distance. As a result, the Z-scheme charge transfer is accelerated due to the synergistic influence of these two factors. Therefore, the optimized CdS/Bi2MoO6 Z-scheme heterojunction possesses significantly enhanced dynamic carrier mobility, thus promoting the conversion of CO2 to CO without the need for additional co-catalysts or sacrificial agents. This optimization yields a remarkable CO selectivity of up to 97%. Meanwhile, the expedited Z-scheme charge transfer mechanism is validated through X-ray photoelectron spectroscopy, Kelvin probe force microscopy, and in situ diffuse reflectance infrared Fourier transform spectroscopy. © 2024 Elsevier Inc.
Keyword ：
Chemical bond Chemical bond CO2 reduction CO2 reduction Internal electric field Internal electric field Photocatalysis Photocatalysis Z-scheme Z-scheme
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| GB/T 7714 | Wu, Y. , Xiao, J. , Yuan, J. et al. Chemically bonded CdS/Bi2MoO6 Z-scheme heterojunction synergises with strong internal electric field for photocatalytic CO2 reduction [J]. | Journal of Colloid and Interface Science , 2024 , 674 : 158-167 . |
| MLA | Wu, Y. et al. "Chemically bonded CdS/Bi2MoO6 Z-scheme heterojunction synergises with strong internal electric field for photocatalytic CO2 reduction" . | Journal of Colloid and Interface Science 674 (2024) : 158-167 . |
| APA | Wu, Y. , Xiao, J. , Yuan, J. , Wang, L. , Luo, S. , Zhang, Z. et al. Chemically bonded CdS/Bi2MoO6 Z-scheme heterojunction synergises with strong internal electric field for photocatalytic CO2 reduction . | Journal of Colloid and Interface Science , 2024 , 674 , 158-167 . |
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Converting CO2 into hydrocarbons using solar energy enables the seamless integration of efficient solar energy utilization and carbon neutrality, presenting an efficacious solution to simultaneously tackle energy and environmental issues. However, challenges arise in controlling the selectivity of reduction products hinder its industrial application due to uncertainties in decisive factors. Given the complexity of the photocatalytic process, it is imperative to improve the understanding of the thermodynamic aspects (including consideration of both redox potential of photocatalysts and light absorption properties, activation of stable CO2 molecules, similarity in reduction potential of products) as well as kinetic obstacles (such as high adsorption potential, significant time disparity between charge separation and transfer, competition from side reactions). This Review offers a comprehensive analysis of the factors that govern product selectivity and explores effective strategies for enhancing catalytic performance based on recent advancements in photocatalytic CO2 reduction to diverse chemical compounds. These profound insights provide invaluable guidance for addressing challenges in practical applications of photocatalytic CO2 conversion.
Keyword ：
Activity Activity CO2 reduction CO2 reduction Photocatalysis Photocatalysis Reactionmechanism Reactionmechanism Selectivity Selectivity
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| GB/T 7714 | Wang, Shuowen , Wang, Jiashun , Wang, Ying et al. Insight into the Selectivity-Determining Step of Various Photocatalytic CO2 Reduction Products by Inorganic Semiconductors [J]. | ACS CATALYSIS , 2024 , 14 (14) : 10760-10788 . |
| MLA | Wang, Shuowen et al. "Insight into the Selectivity-Determining Step of Various Photocatalytic CO2 Reduction Products by Inorganic Semiconductors" . | ACS CATALYSIS 14 . 14 (2024) : 10760-10788 . |
| APA | Wang, Shuowen , Wang, Jiashun , Wang, Ying , Sui, Xiaoyu , Wu, Shuhong , Dai, Wenxin et al. Insight into the Selectivity-Determining Step of Various Photocatalytic CO2 Reduction Products by Inorganic Semiconductors . | ACS CATALYSIS , 2024 , 14 (14) , 10760-10788 . |
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Solar-driven methanation of carbon dioxide (CO2) with water (H2O) has emerged as an important strategy for achieving both carbon neutrality and fuel production. The selective methanation of CO2 was often hindered by the sluggish kinetics and the multiple competition of other C1 byproducts. To overcome this bottleneck, we utilized a biomass synthesis method to synthesize SiC rods and then constructed a direct Z-scheme heterojunction Co3O4/SiC catalyst. The substantial difference in work functions between SiC and Co3O4 served as a significant source of the charge driving force, facilitating the conversion of CO2 to CH4. The high-valent cobalt Co(IV) in Co3O4 acts as an active species to promote efficient dissociation of water. This favorable condition greatly enhanced the likelihood of a high concentration of electrons and protons around a single site on the catalyst surface for CO2 methanation. DFT calculation showed that the energy barrier of CO2 hydrogenation was significantly reduced at the Co3O4/SiC heterojunction interface, which changed the reaction pathway and completely converted the product from CO to CH4. The optimum CH4 evolution rate of Co3O4/SiC samples was 21.3 μmol g-1 h-1 with 100% selectivity. This study has an important guiding significance for the selective regulation of CO2 to CH4 products in photocatalysis applications. © 2024 American Chemical Society.
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| GB/T 7714 | Lin, M. , Cai, Q. , Xiao, Z. et al. Cooperation of Strong Electric Field and H2O Dissociation on Co3O4-Decorated SiC Rods for Photodriven CO2 Methanation with 100% Selectivity [J]. | Inorganic Chemistry , 2024 , 63 (31) : 14591-14601 . |
| MLA | Lin, M. et al. "Cooperation of Strong Electric Field and H2O Dissociation on Co3O4-Decorated SiC Rods for Photodriven CO2 Methanation with 100% Selectivity" . | Inorganic Chemistry 63 . 31 (2024) : 14591-14601 . |
| APA | Lin, M. , Cai, Q. , Xiao, Z. , Chen, H. , Wang, B. , Qiu, C. et al. Cooperation of Strong Electric Field and H2O Dissociation on Co3O4-Decorated SiC Rods for Photodriven CO2 Methanation with 100% Selectivity . | Inorganic Chemistry , 2024 , 63 (31) , 14591-14601 . |
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CO2 is a viable renewable energy source, as global CO2 emissions are perennially increasing. The decomposition of CO2 to CO and O2 through high-temperature cracking of metal oxides via a two-step thermochemical cycle has been an effective strategy to reduce CO2 concentrations in the atmosphere. However, this thermochemical cycle requires a high reaction temperature (1273 K). Hence, in this study, we investigated photothermal CO2 decomposition over three CeO2 catalysts with different morphologies: porous CeO2 nanosheets (2D-CeO2), cubicshaped CeO2 (C-CeO2), and octahedral CeO2 (O-CeO2). The photothermal synergistic effect eliminated the necessity of high temperatures, where light illumination increased the generation of oxygen vacancies and electron transfer to promote CO2 decomposition. The maximum rate of CO production by 2D-CeO2 at 250 degrees C was 69 mu mol g-1h-1, which is significantly higher than those of O-CeO2 (47 mu mol g-1h- 1) and C-CeO2 (19 mu mol g-1h- 1). However, no activity was observed in dark conditions, even at 250 degrees C. In-situ DRIFTS, quasi in-situ EPR, XPS, and Ar-TPD experiments revealed that light irradiation promotes the production of oxygen vacancies on the catalyst surface and generates the intermediate CO2 center dot- species, which cleave the C=O bonds and CO2 conversion, while temperature promotes the adsorption of CO2 on the catalyst surface and facilitates electron transfer. DFT calculations revealed the differences in oxygen vacancy formation and CO2 adsorption among various exposed crystal facets of CeO2. These findings provide new avenues for CO2 decomposition based on the adsorption and activation of CO2 on metal oxide surfaces and the low-temperature synergistic photothermal effect.
Keyword ：
CeO2 CeO2 CO2 decomposition CO2 decomposition Oxygen vacancies Oxygen vacancies Photothermal catalysis Photothermal catalysis
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| GB/T 7714 | Zheng, Duojia , Yue, Xuanyu , Wang, Zhijie et al. Investigation into the photothermal catalytic CO2 decomposition over CeO2 with different morphologies: Behaviors of oxygen vacancies [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 350 . |
| MLA | Zheng, Duojia et al. "Investigation into the photothermal catalytic CO2 decomposition over CeO2 with different morphologies: Behaviors of oxygen vacancies" . | SEPARATION AND PURIFICATION TECHNOLOGY 350 (2024) . |
| APA | Zheng, Duojia , Yue, Xuanyu , Wang, Zhijie , Fan, Shipeng , Zhang, Zizhong , Dai, Wenxin et al. Investigation into the photothermal catalytic CO2 decomposition over CeO2 with different morphologies: Behaviors of oxygen vacancies . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 350 . |
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Photocatalytic methane conversion into liquid oxygenates using O-2 oxidants provides a promising approach for high-value chemicals. The generation of reactive oxygen species and their reaction pathway are key to determine the oxygenate selectivity. Here, an interstitial Zn-i defect ZnO (ZnO(Zn-i)) is developed through thermal decomposition of the ZnO2 precursor. Zn-i favors the O-2 adsorption at a terminal adsorption configuration and induces effectively the conversion O-2 into the desired center dot OOH instead of center dot OH for improving the yield and selectivity of oxygenates. For comparison, O-2 adsorbed in a lateral configuration tends to be converted into excessive center dot OH on the typical Au/ZnO. As a result, ZnO(Zn-i) shows the liquid oxygenates yield of 6080 mu mol g(-1) with 98.6% selectivity, which leads to 10 times lower than Au/ZnO for CO2 release of overoxidation. This work provides a pathway for O-2 adsorption and activation to regulate the photocatalytic CH4 oxidation conversion into liquid oxygenates.
Keyword ：
defects defects interstitial zinc interstitial zinc methane conversion methane conversion oxygen activation oxygen activation selectivity selectivity
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| GB/T 7714 | Xiao, Zhen , Wan, Zhenyu , Zhang, Jiangjie et al. Interstitial Zinc Defects Enriched ZnO Tuning O2 Adsorption and Conversion Pathway for Superior Photocatalytic CH4 Oxygenation [J]. | ACS CATALYSIS , 2024 . |
| MLA | Xiao, Zhen et al. "Interstitial Zinc Defects Enriched ZnO Tuning O2 Adsorption and Conversion Pathway for Superior Photocatalytic CH4 Oxygenation" . | ACS CATALYSIS (2024) . |
| APA | Xiao, Zhen , Wan, Zhenyu , Zhang, Jiangjie , Jiang, Jianing , Li, Dongmiao , Shen, Jinni et al. Interstitial Zinc Defects Enriched ZnO Tuning O2 Adsorption and Conversion Pathway for Superior Photocatalytic CH4 Oxygenation . | ACS CATALYSIS , 2024 . |
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