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学者姓名：张子重
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Abstract ：
The electrocatalytic conversion of inert CO2 to value-added chemical fuels powered by renewable energy is one of the benchmark approaches to address excessive carbon emissions and achieve carbon-neutral energy restructuring. However, the adsorption/activation of supersymmetric CO2 is facing insurmountable challenges that constrain its industrial-scale applications. Here, this theory-guided study confronts these challenges by leveraging the synergies of bimetallic sites and defect engineering, where pyrochlore-type semiconductor A(2)B(2)O(7) is employed as research platform and the conversion of CO2-to-HCOOH as the model reaction. Specifically, defect engineering intensified greatly the chemisorption-induced CO2 polarization via the bimetallic coordination, thermodynamically beneficial to the HCOOH production via the *HCO2 intermediate. The optimal V-BSO-430 electrocatalyst with abundant surface oxygen vacancies achieved a superior HCOOH yield of 116.7 mmol h(-1) cm(-2) at -1.2 V-RHE, rivalling the incumbent similar reaction systems. Furthermore, the unique catalytic unit featured with a Bi-1-Sn-Bi-2 triangular structure, which is reconstructed by defect engineering, and altered the pathway of CO2 adsorption and activation to allow the preferential affinity of the suspended O atom in *HCO2 to H. As a result, V-BSO-430 gave an impressive FEHCOOH of 93% at -1.0 V-RHE. This study held promises for inspiring the exploration of bimetallic materials from the massive semiconductor database.
Keyword ：
A(2)B(2)O(7) A(2)B(2)O(7) bimetallic sites bimetallic sites CO2 reduction CO2 reduction electrocatalysis electrocatalysis pyrochlore pyrochlore
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| GB/T 7714 | Zhao, Jiwu , Wang, Jiashun , Xue, Lan et al. Surface Oxygen Defect Engineering of A2B2O7 Pyrochlore Semiconductors Boosts the Electrocatalytic Reduction of CO2-to-HCOOH [J]. | SMALL , 2024 , 20 (38) . |
| MLA | Zhao, Jiwu et al. "Surface Oxygen Defect Engineering of A2B2O7 Pyrochlore Semiconductors Boosts the Electrocatalytic Reduction of CO2-to-HCOOH" . | SMALL 20 . 38 (2024) . |
| APA | Zhao, Jiwu , Wang, Jiashun , Xue, Lan , Wang, Ying , Wen, Na , Huang, Haowei et al. Surface Oxygen Defect Engineering of A2B2O7 Pyrochlore Semiconductors Boosts the Electrocatalytic Reduction of CO2-to-HCOOH . | SMALL , 2024 , 20 (38) . |
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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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Solar-powered photocatalytic water splitting for hydrogen evolution presents a promising solution to the energy crisis and contemporary environmental challenges. Herein, a Z-scheme ZnS/LaTiO2N heterojunction composite, incorporating zinc vacancies, has been successfully synthesized to enable photocatalytic hydrogen evolution under visible-light illumination. The optimized ZnS(VZn)/LaTiO2N composite demonstrates a hydrogen evolution activity 13 times higher than that of individual ZnS(VZn). The heterojunction between ZnS and LaTiO2N, in conjunction with zinc vacancies, expands the photoresponse spectrum and facilitates the spatial separation and transfer of photogenerated carriers. Consequently, this synergy significantly enhances the performance of photocatalytic hydrogen evolution. The collaborative action of the Z-scheme heterojunction and zinc vacancies paves the way for innovative approaches in designing future high-efficiency photocatalysts.
Keyword ：
LaTiO2N LaTiO2N Photocatalytic H 2 evolution Photocatalytic H 2 evolution ZnS(VZn) ZnS(VZn) Z-scheme heterojunction Z-scheme heterojunction
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| GB/T 7714 | Yu, Jiaqi , Qi, Jinwei , Lin, Nansong et al. Zinc-vacancy mediated Z-scheme photocatalyst of ZnS/LaTiO2N for hydrogen evolution under visible-light [J]. | JOURNAL OF ALLOYS AND COMPOUNDS , 2024 , 976 . |
| MLA | Yu, Jiaqi et al. "Zinc-vacancy mediated Z-scheme photocatalyst of ZnS/LaTiO2N for hydrogen evolution under visible-light" . | JOURNAL OF ALLOYS AND COMPOUNDS 976 (2024) . |
| APA | Yu, Jiaqi , Qi, Jinwei , Lin, Nansong , Zhang, Zizhong , Ji, Tao , Su, Wenyue . Zinc-vacancy mediated Z-scheme photocatalyst of ZnS/LaTiO2N for hydrogen evolution under visible-light . | JOURNAL OF ALLOYS AND COMPOUNDS , 2024 , 976 . |
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1,8-naphthalene anhydride (1,8-NA) is a common polycyclic aromatic hydrocarbons (PAHs) which are the most important light absorbed-organic aerosols (BrC) in atmospheric. 1,8-NA can generate different ROSs (.OH, .O2- , H2O2, 1O2) under the visible light irradiation. According to the results of DFT simulation and band structure analysis, 1,8-NA has the semiconductor characteristic, and the electrons of it can be excited from acid anhydride part to naphthalene ring part. Meanwhile, a built-in electric field exists between the acid anhydride and the naphthalene ring because of the molecular polarization of 1,8-NA. This electric field could promote the separation and migration of carriers. Therefore, electrons can easily be transferred to O2 and produce ROS. The properties and mechanism of photocatalytic O2 activation by atmospheric aerosol component 1, 8-NA were studied for the first time, which provided good support for further understanding of atmospheric photochemical mechanism.
Keyword ：
Built-in electric field Built-in electric field internal polar molecule internal polar molecule Organic aerosol Organic aerosol Reactive oxygen species Reactive oxygen species
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| GB/T 7714 | Dong, Tingting , Dong, Guohui , Li, Yuxin et al. Photocatalytic O2 activation carried out by organic aerosol: A case study of 1, 8-naphthalic anhydride [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 349 . |
| MLA | Dong, Tingting et al. "Photocatalytic O2 activation carried out by organic aerosol: A case study of 1, 8-naphthalic anhydride" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 349 (2024) . |
| APA | Dong, Tingting , Dong, Guohui , Li, Yuxin , Zhang, Zizhong . Photocatalytic O2 activation carried out by organic aerosol: A case study of 1, 8-naphthalic anhydride . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 349 . |
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Efficient photocatalytic reduction of CO2 to high-calorific-value CH4, an ideal target product, is a blueprint for C-1 industry relevance and carbon neutrality, but it also faces great challenges. Herein, we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst, which are prepared via a facile impregnation-reduction method, featuring an optimized local electronic structure. It exhibits a superior photocatalytic carbon-based products yield of 30.0 mu mol g(-1) h(-1) and achieves a record CH4 selectivity of up to 94.3%, which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and selectivity. Specifically, the synergistic effects of directional migration of photogenerated electrons and strong pi-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO2 -> CH4 pathway. This study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.
Keyword ：
artificial synthesis of CH4 artificial synthesis of CH4 electronic structure optimization electronic structure optimization Fe species cocatalyst Fe species cocatalyst photocatalytic CO2 reduction photocatalytic CO2 reduction SiC SiC
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| GB/T 7714 | Lin, Qianying , Zhao, Jiwu , Zhang, Pu et al. Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation [J]. | CARBON ENERGY , 2024 , 6 (1) . |
| MLA | Lin, Qianying et al. "Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation" . | CARBON ENERGY 6 . 1 (2024) . |
| APA | Lin, Qianying , Zhao, Jiwu , Zhang, Pu , Wang, Shuo , Wang, Ying , Zhang, Zizhong et al. Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation . | CARBON ENERGY , 2024 , 6 (1) . |
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Photocatalytic selective oxidation of alcohols into aldehydes and H2 is a green strategy for obtaining both valueadded chemicals and clean energy. Herein, a dual-purpose ZnIn2S4@CdS photocatalyst was designed and constructed for efficient catalyzing benzyl alcohol (BA) into benzaldehyde (BAD) with coupled H2 evolution. To address the deep-rooted problems of pure CdS, such as high recombination of photogenerated carriers and severe photo-corrosion, while also preserving its superiority in H2 production, ZnIn2S4 with a suitable band structure and adequate oxidizing capability was chosen to match CdS by constructing a coupled reaction. As designed, the photoexcited holes (electrons) in the CdS (ZnIn2S4) were spatially separated and transferred to the ZnIn2S4 (CdS) by electrostatic pull from the built-in electric field, leading to expected BAD production (12.1 mmol g-1 h-1) at the ZnIn2S4 site and H2 generation (12.2 mmol g-1 h-1) at the CdS site. This composite photocatalyst also exhibited high photostability due to the reasonable hole transfer from CdS to ZnIn2S4. The experimental results suggest that the photocatalytic transform of BA into BAD on ZnIn2S4@CdS is via a carbon-centered radical mechanism. This work may extend the design of advanced photocatalysts for more chemicals by replacing H2 evolution with N2 fixation or CO2 reduction in the coupled reactions.
Keyword ：
Hydrogen evolution Hydrogen evolution Regulated catalytic sites Regulated catalytic sites Selective oxidation Selective oxidation Type-II heterojunction Type-II heterojunction ZnIn 2 S 4 @CdS ZnIn 2 S 4 @CdS
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| GB/T 7714 | Yang, Lifang , Guo, Jiao , Chen, Siyan et al. Tailoring the catalytic sites by regulating photogenerated electron/hole pairs separation spatially for simultaneous selective oxidation of benzyl alcohol and hydrogen evolution [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 659 : 776-787 . |
| MLA | Yang, Lifang et al. "Tailoring the catalytic sites by regulating photogenerated electron/hole pairs separation spatially for simultaneous selective oxidation of benzyl alcohol and hydrogen evolution" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 659 (2024) : 776-787 . |
| APA | Yang, Lifang , Guo, Jiao , Chen, Siyan , Li, Aoqi , Tang, Jun , Guo, Ning et al. Tailoring the catalytic sites by regulating photogenerated electron/hole pairs separation spatially for simultaneous selective oxidation of benzyl alcohol and hydrogen evolution . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 659 , 776-787 . |
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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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