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节能减排 4

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Pt–Ba–Ce/γ-Al2O3 催化剂，物理化学性质，NOx存储和还原，NOx 排放，H2 还原剂 1

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互耦；多输入多输出；天线阵列；超表面；去耦 1

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In situ DRIFTS study of photocatalytic CO 2 reduction under UV irradiation

Jeffrey C. S. WU, Chao-Wei HUANG,

《化学科学与工程前沿（英文）》 2010年 第4卷 第2期   页码 120-126 doi: 10.1007/s11705-009-0232-3

摘要： Photocatalytic reduction of CO on TiO and Cu/TiO photocatalysts was studied by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) under UV irradiation. The photocatalysts were prepared by sol-gel method via controlled hydrolysis of titanium (IV) butoxide. Copper precursor was loaded onto TiO during sol-gel procedure. A large amount of adsorbed HO and surface OH groups was detected at 25°C on the TiO photocatalyst after being treated at 500°C under air stream. Carbonate and bicarbonate were formed rapidly due to the reaction of CO with oxygen-vacancy and OH groups, respectively, on TiO surface upon CO adsorption. The IR spectra indicated that, under UV irradiation, gas-phase CO further combined with oxygen-vacancy and OH groups to produce more carbonate or bicarbonate. The weak signals of reaction intermediates were found on the IR spectra, which were due to the slow photocatalytic CO reduction on photocatalysts. Photogenerated electrons merge with H ions to form H atoms, which progressively reduce CO to form formic acid, dioxymethylene, formaldehyde and methoxy as observed in the IR spectra. The well-dispersed Cu, acting as the active site significantly increases the amount of formaldehyde and dioxymethylene, thus promotes the photoactivity of CO reduction on Cu/TiO. A possible mechanism of the photocatalytic CO reduction is proposed based on these intermediates and products on the photocatalysts.

关键词： irradiation     oxygen-vacancy     Photocatalytic reduction     Carbonate     butoxide    

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Efficient elimination of environmental pollutants through sorption-reduction and photocatalytic degradation

Njud S. Alharbi, Baowei Hu, Tasawar Hayat, Samar Omar Rabah, Ahmed Alsaedi, Li Zhuang, Xiangke Wang

《化学科学与工程前沿（英文）》 2020年 第14卷 第6期   页码 1124-1135 doi: 10.1007/s11705-020-1923-z

摘要： With the rapid development of industrial, large amounts of different inorganic and organic pollutants are released into the natural environments. The efficient elimination of environmental pollutants, i.e., photocatalytic degradation of persistent organic pollutants into nontoxic organic/inorganic chemicals, solidification or sorption-reduction of heavy metal ions, is crucial to protect the environment. Nanomaterials with large surface area, active sites and abundant functional groups could form strong surface complexes with different kinds of pollutants and thereby could efficiently eliminate the pollutants from the aqueous solutions. In this review, we mainly focused on the recent works about the synthesis of nanomaterials and their applications in the efficient elimination of different organic and inorganic pollutants from wastewater and discussed the interaction mechanism from batch experimental results, the advanced spectroscopy techniques and theoretical calculations. The adsorption and the photocatalytic reduction of organic pollutants and the sorption/reduction of heavy metal ions are generally considered as the main methods to decrease the concentration of pollutants in the natural environment. This review highlights a new way for the real applications of novel nanomaterials in environmental pollution management, especially for the undergraduate students to understand the recent works in the elimination of different kinds of inorganic and organic chemicals in the natural environmental pollution management.

关键词： nanomaterials     sorption-reduction     photocatalytic degradation     organic pollutants     heavy metal ions    

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Photocatalytic reduction of carbon dioxide by titanium oxide-based semiconductors to produce fuels

Xi CHEN, Fangming JIN

《能源前沿（英文）》 2019年 第13卷 第2期   页码 207-220 doi: 10.1007/s11708-019-0628-9

摘要： To tackle the crisis of global warming, it is imperative to control and mitigate the atmospheric carbon dioxide level. Photocatalytic reduction of carbon dioxide into solar fuels furnishes a gratifying solution to utilize and reduce carbon dioxide emission and simultaneously generate renewable energy to sustain the societies. So far, titanium oxide-based semiconductors have been the most prevalently adopted catalysts in carbon dioxide photoreduction. This mini-review provides a general summary of the recent progresses in titanium oxide-catalyzed photocatalytic reduction of carbon dioxide. It first illustrates the use of structural engineering as a strategy to adjust and improve the catalytic performances. Then, it describes the introduction of one/two exogenous elements to modify the photocatalytic activity and/or selectivity. Lastly, it discusses multi-component hybrid titanium oxide composites.

关键词： photocatalysis     carbon dioxide reduction     semiconductors     titanium oxide     renewable fuels    

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ZnFe2O4 deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO2 in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

《化学科学与工程前沿（英文）》 2017年 第11卷 第2期   页码 197-204 doi: 10.1007/s11705-016-1606-y

摘要： ZnFe O -BiOCl composites were prepared by both hydrothermal and direct precipitation processes and the structures and properties of the samples were characterized by various instrumental techniques. The samples were then used as catalysts for the photocatalytic reduction of CO in cyclohexanol under ultraviolet irradiation to give cyclohexanone (CH) and cyclohexyl formate (CF). The photocatalytic CO reduction activities over the hydrothermally prepared ZnFe O -BiOCl composites were higher than those over the directly-precipitated composites. This is because compared to the direct-precipitation sample, the ZnFe O nanoparticles in the hydrothermal sample were smaller and more uniformly distributed on the surface of BiOCl and so more heterojunctions were formed. Higher CF and CH yields were obtained for the pure BiOCl and BiOCl composite samples with more exposed (001) facets than for the samples with more exposed (010) facets. This is due to the higher density of oxygen atoms in the exposed (001) facets, which creates more oxygen vacancies, and thereby improves the separation efficiency of the electron-hole pairs. More importantly, irradiation of the (001) facets with ultraviolet light produces photo-generated electrons which is helpful for the reduction of CO to ·CO . The mechanism for the photocatalytic reduction of CO in cyclohexanol over ZnFe O -BiOCl composites with exposed (001) facets involves electron transfer and carbon radical formation.

关键词： reduction of CO2     cyclohexanol     ZnFe2O4 deposited BiOCl     facet     composite photocatalyst    

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Newly-modeled graphene-based ternary nanocomposite for the magnetophotocatalytic reduction of CO2 with

《化学科学与工程前沿（英文）》 2022年 第16卷 第10期   页码 1438-1459 doi: 10.1007/s11705-022-2166-y

摘要： The development of CO2 into hydrocarbon fuels has emerged as a green method that could help mitigate global warning. The novel structured photocatalyst is a promising material for use in a photocatalytic and magneto-electrochemical method that fosters the reduction of CO2 by suppressing the recombination of electron−hole pairs and effectively transferring the electrons to the surface for the chemical reaction of CO2 reduction. In our study, we have developed a novel-structured AgCuZnS2–graphene–TiO2 to analyze its catalytic activity toward the selective evolution of CO2. The selectivity of each nanocomposite substantially enhanced the activity of the AgCuZnS2–graphene–TiO2 ternary nanocomposite due to the successful interaction, and the selectivity of the final product was improved to a value 3 times higher than that of the pure AgCuZnS2 and 2 times higher than those of AgCuZnS2–graphene and AgCuZnS2–TiO2 under ultra-violet (UV)-light (λ = 254 nm) irradiation in the photocatalytic process. The electrochemical CO2 reduction test was also conducted to analyze the efficacy of the AgCuZnS2–graphene–TiO2 when used as a working electrode in laboratory electrochemical cells. The electrochemical process was conducted under different experimental conditions, such as various scan rates (mV·s–1), under UV-light and with a 0.07 T magnetic-core. The evolution of CO2 substantially improved under UV-light (λ = 254 nm) and with 0.07 T magnetic-core treatment; these improvements were attributed to the facts that the UV-light activated the electron-transfer pathway and the magnetic core controlled the pathway of electron-transmission/prevention to protect it from chaotic electron movement. Among all tested nanocomposites, AgCuZnS2–graphene–TiO2 absorbed the CO2 most strongly and showed the best ability to transfer the electron to reduce the CO2 to methanol. We believe that our newly-modeled ternary nanocomposite opens up new opportunities for the evolution of CO2 to methanol through an electrochemical and photocatalytic process.

关键词： ternary nanocomposite     photocatalytic     electrochemical CO2 reduction     UV-light     magnetic core    

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Graphene-like -BN supported polyhedral NiS/NiS nanocrystals with excellent photocatalytic performance

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1537-1549 doi: 10.1007/s11705-021-2094-2

摘要： Human health is deteriorating due to the effluent containing heavy metal ions and organic dyes. Hence, photoreduction of Cr(VI) to Cr(III) and degradation of rhodamine B (RhB) using a novel photocatalyst is particularly important. In this work, h-BN/NiS2/NiS composites were prepared via a simple solvothermal method and a double Z-scheme heterojunction was constructed for efficiently removing RhB and Cr(VI). The 7 wt-% h-BN/NiS2/NiS composites were characterized via a larger specific surface area (15.12 m2·g–1), stronger light absorption capacity, excellent chemical stability, and high yield of electrons and holes. The experimental result indicated that the photoreduction efficiency of the 7 wt-% h-BN/NiS2/NiS photocatalyst achieved 98.5% for Cr(VI) after 120 min, which was about 3 times higher than that of NiS2/NiS (34%). However, the removal rate of RhB by the 7 wt-% h-BN/NiS2/NiS photocatalyst reached 80%. This is due to the double Z-scheme heterojunction formed between NiS2/NiS and h-BN, which improved the charge separation efficiency and transmission efficiency. Besides, the influence of diverse photogenerated electron and hole scavengers upon the photoreduction of Cr(VI) was studied, the results indicated that graphene-like h-BN promoted transportation of photoinduced charges on the surface of the h-BN/NiS2/NiS photocatalyst via the interfacial effects.

关键词： graphene-like h-BN     h-BN/NiS2/NiS composites     photocatalysis     Cr(VI) reduction     degradation of RhB    

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Review on design and evaluation of environmental photocatalysts

Xin Li, Jun Xie, Chuanjia Jiang, Jiaguo Yu, Pengyi Zhang

《环境科学与工程前沿（英文）》 2018年 第12卷 第5期 doi: 10.1007/s11783-018-1076-1

摘要：

Fundamentals on the photocatalytic degradation were systematically summarized.

Charge carrier dynamics for the photocatalytic degradation were reviewed.

Adsorption and photodegradation kinetics of reactants were highlighted.

The mechanism aspects, including O2 reduction, reactive oxidation species and key intermediates were also addressed.

Selectivity and stability of semiconductors for photodegradation were clarified.

关键词： Photocatalytic degradation     Environmental remediation     Charge carrier dynamics     Reactive oxygen species     O2 reduction    

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preparation of Ag@AgCl/Bio-veins composites and their photocatalytic activity and recyclability

《化学科学与工程前沿（英文）》 2023年 第17卷 第7期   页码 906-917 doi: 10.1007/s11705-022-2273-9

摘要： The industrial application of nano-photocatalysts in wastewater treatment has been severely restricted for a long time due to their difficult separation, poor reusability, and low efficiency. In this work, a facile strategy was proposed to enhance the photocatalytic activity and recovery performance of Ag@AgCl nanocatalysts. Biological veins (Bio-veins) with a unique 3D porous construction were used as carriers for the in-situ growth of Ag@AgCl nanoparticles. Scanning electron microscopy results showed that the Ag@AgCl nanoparticles were uniformly loaded on the surface and interior of the Bio-veins, and the size of the Ag@AgCl nanoparticles immobilized on the Bio-veins (50–300 nm) was significantly smaller than Ag@AgCl obtained by the co-precipitation method (1–3 μm). The Bio-veins played a vital role in the photocatalysis reaction system. The degradation efficiency of the Ag@AgCl/Bio-veins(CI4) was up to 3.50 times as high as pure Ag@AgCl. Furthermore, the composites also exhibited excellent recyclability and stability under both visible and solar light. This work provided a suitable strategy for nano-photocatalysts for practical application and may also offer new possibilities for the high-value utilization of biomass materials.

关键词： Ag@AgCl     biological veins     photocatalytic activity     recyclability    

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Enhanced photocatalytic water splitting with surface defective SrTiO

Junying LIU, Zhidong WEI, Wenfeng SHANGGUAN

《能源前沿（英文）》 2021年 第15卷 第1期   页码 700-709 doi: 10.1007/s11708-021-0735-2

摘要： Surface reconstructed SrTiO nanocrystals were synthesized by a thermal treatment process in presence of NaBH and SrTiO nanocrystals. The surface reconstruction of SrTiO nanocrystals is attributed to the introduction of surface oxygen vacancies or Ti sites (such as Ti and Ti ) during the hydrogenation treatment process. The light absorption and the charge transfer ability of SrTiO nanocrystals are simultaneously enhanced due to surface oxygen vacancies or Ti sites (such as Ti and Ti ), which are beneficial to photocatalytic water splitting. Meanwhile, these defects also change the redox potential of the photocatalysts. Since there existed a synergistic effect between the three, the ratio of hydrogen to oxygen production was also regulated.

关键词： SrTiO3     surface reconstruction     oxygen vacancies     photocatalytic water splitting    

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Design and synthesis of ZnCoO/CdS for substantially improved photocatalytic hydrogen production

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 606-616 doi: 10.1007/s11705-022-2233-4

摘要： In this study, the hydrogen evolution performance of CdS nanorods is improved using ZnCo2O4. ZnCo2O4 nanospheres are synthesized using the hydrothermal and calcination methods, and CdS nanorods are synthesized using the solvothermal method. From the perspective of morphology, numerous CdS nanorods are anchored on the ZnCo2O4 microspheres. According to the experimental results of photocatalytic hydrogen evolution, the final hydrogen evolution capacity of 7417.5 μmol∙g–1∙h–1 is slightly more than two times that of the single CdS, which proves the feasibility of our study. Through various characterization methods, it is proved that the composite sample has suitable optoelectronic properties. In addition, ZnCo2O4 itself exhibits good conductivity and low impedance, which shortens the charge-transfer path. Overall, the introduction of ZnCo2O4 expands the adsorption range of light and improves the performance of photocatalytic hydrogen evolution. This design can provide reference for developing high-efficiency photocatalysts.

关键词： ZnCo2O4 nanosphere     CdS nanorods     photocatalytic hydrogen evolution    

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Theoretical study on flow and radiation in tubular solar photocatalytic reactor

《能源前沿（英文）》 2021年 第15卷 第3期   页码 687-699 doi: 10.1007/s11708-021-0773-9

摘要： In this paper, based on the mixture flow model, an optimized six-flux model is first established and applied to the tubular solar photocatalytic reactor. Parameters influencing photocatalyst distribution and radiation distribution at the reactor outlet, viz. catalyst concentration and circulation speed, are also analyzed. It is found that, at the outlet of the reactor, the optimized six-flux model has better performances (the energy increase by 1900% and 284%, respectively) with a higher catalyst concentration (triple) and a lower speed (one third).

关键词： photocatalytic hydrogen photoreactor     nume- rical simulation     solar energy     flow model     radiation model    

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Decoration of CdMoO micron polyhedron with Pt nanoparticle and their enhanced photocatalytic performance

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1949-1961 doi: 10.1007/s11705-023-2360-6

摘要： This study aimed to prepare and apply a novel Pt/CdMoO4 composite photocatalyst for photocatalytic N2 fixation and tetracycline degradation. The Pt/CdMoO4 composite was subjected to comprehensive investigation on the morphology, structure, optical properties, and photoelectric chemical properties. The results demonstrate the dispersion of Pt nanoparticles on the CdMoO4 surface. Close contact between CdMoO4 and Pt was observed, resulting in the formation of a heterojunction structure at their contact region. Density functional theory calculation and Mott-Schottky analysis revealed that Pt possesses a higher work function value than CdMoO4, resulting in electron drift from CdMoO4 to Pt and the formation of a Schottky barrier. The presence of this barrier increases the separation efficiency of electron-hole pairs, thereby improving the performance of the Pt/CdMoO4 composite in photocatalysis. When exposed to simulated sunlight, the optimal Pt/CdMoO4 catalyst displayed a photocatalytic nitrogen fixation rate of 443.7 μmol·L‒1·g‒1·h‒1, which is 3.2 times higher than that of pure CdMoO4. In addition, the composite also exhibited excellent performance in tetracycline degradation, with hole and superoxide species identified as the primary reactive species. These findings offer practical insights into designing and synthesizing efficient photocatalysts for photocatalytic nitrogen fixation and antibiotics removal.

关键词： photocatalytic N2 fixation     Pt/CdMoO4     tetracycline degradation     Schottky barrier    

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growth of a-few-layered MoS on CdS nanorod for high efficient photocatalytic H production

《能源前沿（英文）》 2021年 第15卷 第3期   页码 752-759 doi: 10.1007/s11708-021-0779-3

摘要： An ultrathin MoS2 was grown on CdS nanorod by a solid state method using sulfur powder as sulfur source for photocatalytic H2 production. The characterization result reveals that the ultrathin MoS2 nanosheets loaded on CdS has a good contact state. The photoelectrochemical result shows that MoS2 not only are beneficial for charge separation, but also works as active sites, thus enhancing photocatalytic activity. Compared with pure CdS, the photocatalytic activity of MoS2 loaded CdS was significantly improved. The hydrogen evolution rate on m(MoS2): m(CdS) = 1: 50 (m is mass) reaches 542 μmol/h, which is 6 times of that on pure CdS (92 μmol/h). This work provides a new design for photocatalysts with high photocatalytic activities and provides a deeper understanding of the effect of MoS2 on enhancing photocatalytic activity.

关键词： photocatalytic H2 production     CdS     MoS2 cocatalyst     charge separation    

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grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

《能源前沿（英文）》 2021年 第15卷 第3期   页码 721-731 doi: 10.1007/s11708-021-0766-8

摘要： Titanium nitride (TiN) decorated N-doped titania (N-TiO2) composite (TiN/N-TiO2) is fabricated via an in situ nitridation using a hydrothermally synthesized TiO2 and melamine (MA) as raw materials. After the optimization of the reaction condition, the resultant TiN/N-TiO2 composite delivers a hydrogen evolution activity of up to 703 μmol/h under the full spectrum irradiation of Xe-lamp, which is approximately 2.6 and 32.0 times more than that of TiO2 and TiN alone, respectively. To explore the underlying photocatalytic mechanism, the crystal phase, morphology, light absorption, energy band structure, element composition, and electrochemical behavior of the composite material are characterized and analyzed. The results indicate that the superior activity is mainly caused by the in situ formation of plasmonic TiN and N-TiO2 with intimate interface contact, which not only extends the spectral response range, but also accelerates the transfer and separation of the photoexcited hot charge carrier of TiN. The present study provides a fascinating approach to in situ forming nonmetallic plasmonic material/N-doped TiO2 composite photocatalysts for high-efficiency water splitting.

关键词： photocatalytic H2 evolution     TiN/N-TiO2 composite     plasmonic effect     in-situ nitridation    

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Synthesis of TiO2 nano-particles and their photocatalytic activity for formaldehyde and methyl orange

XIAO Xinyan, ZHANG Huiping, CHEN Huanqin, LIAO Dongliang

《化学科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 178-183 doi: 10.1007/s11705-007-0033-5

摘要： TiO nano-particles were synthesized by sol-gel technique and characterized by X-ray diffractometer (XRD) and transmission electron microscope (TEM). Their photocatalytic activities for formaldehyde (FA) and methyl orange (MO) degradation were tested using degradation rate (η) as an evaluation index. Based on the orthogonal test results, the optimal condition for TiO preparation was obtained. Results showed that particle sizes were in the range of 10 40 nm, and that prepared TiO had better photocatalytic activity than P25. A simplified model was developed to evaluate the apparent quantum efficiency (Φapp) of this photocatalytic reaction system.

关键词： prepared     photocatalytic activity     apparent     photocatalytic     orthogonal    

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标题 作者 时间 类型 操作

In situ DRIFTS study of photocatalytic CO 2 reduction under UV irradiation

Jeffrey C. S. WU, Chao-Wei HUANG,

期刊论文

Efficient elimination of environmental pollutants through sorption-reduction and photocatalytic degradation

Njud S. Alharbi, Baowei Hu, Tasawar Hayat, Samar Omar Rabah, Ahmed Alsaedi, Li Zhuang, Xiangke Wang

期刊论文

Photocatalytic reduction of carbon dioxide by titanium oxide-based semiconductors to produce fuels

Xi CHEN, Fangming JIN

期刊论文

ZnFe2O4 deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO2 in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

期刊论文

Newly-modeled graphene-based ternary nanocomposite for the magnetophotocatalytic reduction of CO2 with

期刊论文

Graphene-like -BN supported polyhedral NiS/NiS nanocrystals with excellent photocatalytic performance

期刊论文

Review on design and evaluation of environmental photocatalysts

Xin Li, Jun Xie, Chuanjia Jiang, Jiaguo Yu, Pengyi Zhang

期刊论文

preparation of Ag@AgCl/Bio-veins composites and their photocatalytic activity and recyclability

期刊论文

Enhanced photocatalytic water splitting with surface defective SrTiO

Junying LIU, Zhidong WEI, Wenfeng SHANGGUAN

期刊论文

Design and synthesis of ZnCoO/CdS for substantially improved photocatalytic hydrogen production

期刊论文

Theoretical study on flow and radiation in tubular solar photocatalytic reactor

期刊论文

Decoration of CdMoO micron polyhedron with Pt nanoparticle and their enhanced photocatalytic performance

期刊论文

growth of a-few-layered MoS on CdS nanorod for high efficient photocatalytic H production

期刊论文

grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

期刊论文

Synthesis of TiO2 nano-particles and their photocatalytic activity for formaldehyde and methyl orange

XIAO Xinyan, ZHANG Huiping, CHEN Huanqin, LIAO Dongliang

期刊论文