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Decoration of CdMoO micron polyhedron with Pt nanoparticle and their enhanced photocatalytic performancein N fixation and water purification

《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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Cu-doped Bi/Bi<sub>2sub>WO<sub>6sub> catalysts for efficient N<sub>2sub> fixation by photocatalysis

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1412-1422 doi: 10.1007/s11705-023-2312-1

摘要： In this paper, Cu-doped Bi2WO6 was synthesized via a solvothermal method and applied it in photocatalytic N2 immobilization. Characterization results showed the presence of a small amount of metallic Bi in the photocatalyst, indicating that the synthesized photocatalyst is actually Bi/Cu-Bi2WO6 composite. The doped Cu had a valence state of +2 and most likely substituted the position of Bi3+. The introduced Cu did not affect the metallic Bi content, but mainly influenced the energy band structure of Bi2WO6. The band gap was slightly narrowed, the conduction band was elevated, and the work function was reduced. The reduced work function improved the transfer and separation of charge carriers, which mainly caused the increased photoactivity. The optimized NH3 generation rates of Bi/Cu-Bi2WO6 reached 624 and 243 μmol·L–1·g–1·h–1 under simulated solar and visible light, and these values were approximately 2.8 and 5.9 times higher those of Bi/Bi2WO6, respectively. This research provides a method for improving the photocatalytic N2 fixation and may provide more information on the design and preparation of heteroatom-doped semiconductor photocatalysts for N2-to-NH3 conversion.

关键词： Bi2WO6     Cu doping     work function     photocatalytic N2 fixation     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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Cyanobacterial photo-driven mixotrophic metabolism and its advantages for biosynthesis

Ni Wan,Mary Abernathy,Joseph Kuo-Hsiang Tang,Yinjie J. Tang,Le You

《化学科学与工程前沿（英文）》 2015年 第9卷 第3期   页码 308-316 doi: 10.1007/s11705-015-1521-7

摘要： Cyanobacterium offers a promising chassis for phototrophic production of renewable chemicals. Although engineered cyanobacteria can achieve similar product carbon yields as heterotrophic microbial hosts, their production rate and titer under photoautotrophic conditions are 10 to 100 folds lower than those in fast growing Cyanobacterial factories face three indomitable bottlenecks. First, photosynthesis has limited ATP and NADPH generation rates. Second, CO fixation by ribulose-1,5-bisphosphate carboxylase/oxygenase (RuBisCO) has poor efficiency. Third, CO mass transfer and light supply are deficient within large photobioreactors. On the other hand, cyanobacteria may employ organic substrates to promote phototrophic cell growth, N fixation, and metabolite synthesis. The photo-fermentations show enhanced photosynthesis, while CO loss from organic substrate degradation can be reused by the Calvin cycle. In addition, the plasticity of cyanobacterial pathways (e.g., oxidative pentose phosphate pathway and the TCA cycle) has been recently revealed to facilitate the catabolism. The use of cyanobacteria as “green ” could be a promising route to develop robust photo-biorefineries.

关键词： CO2 mass transfer     N2 fixation     photosystem     RuBisCO     the TCA cycle    

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In-MOF-derived In<sub>2sub>S<sub>3sub>/Bi<sub>2sub>S<sub>3sub> heterojunction for enhanced photocatalytic

《能源前沿（英文）》 2023年 第17卷 第5期   页码 654-663 doi: 10.1007/s11708-023-0885-5

摘要： Transition metal sulfides are commonly studied as photocatalysts for water splitting in solar-to-fuel conversion. However, the effectiveness of these photocatalysts is limited by the recombination and restricted light absorption capacity of carriers. In this paper, a broad spectrum responsive In2S3/Bi2S3 heterojunction is constructed by in-situ integrating Bi2S3 with the In2S3, derived from an In-MOF precursor, via the high-temperature sulfidation and solvothermal methods. Benefiting from the synergistic effect of wide-spectrum response, effective charge separation and transfer, and strong heterogeneous interfacial contacts, the In2S3/Bi2S3 heterojunction demonstrates a rate of 0.71 mmol/(g∙h), which is 2.2 and 1.7 times as much as those of In2S3 (0.32 mmol/(g∙h) and Bi2S3 (0.41 mmol/(g∙h)), respectively. This paper provides a novel idea for rationally designing innovative heterojunction photocatalysts of transition metal sulfides for photocatalytic hydrogen production.

关键词： photocatalytic hydrogen production     wide-spectrum response     metal sulfides     MOFs derivative     heterogeneous interfacial contact    

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Interfacial charge transfer and photocatalytic activity in a reverse designed BiO/TiO core-shell

《能源前沿（英文）》 2021年 第15卷 第3期   页码 732-743 doi: 10.1007/s11708-021-0772-x

摘要： In this study, the electronic and photocatalytic properties of core-shell heterojunctions photocatalysts with reversible configuration of TiO2 and Bi2O3 layers were studied. The core-shell nanostructure, obtained by efficient control of the sol-gel polymerization and impregnation method of variable precursors of semiconductors, makes it possible to study selectively the role of the interfacial charge transfer in each configuration. The morphological, optical, and chemical composition of the core-shell nanostructures were characterized by high-resolution transmission electron microscopy, UV-visible spectroscopy and X-ray photoelectron spectroscopy. The results show the formation of homogenous TiO2 anatase and Bi2O3 layers with a thickness of around 10 and 8 nm, respectively. The interfacial charge carrier dynamic was tracked using time resolved microwave conductivity and transition photocurrent density. The charge transfer, their density, and lifetime were found to rely on the layout layers in the core-shell nanostructure. In optimal core-shell design, Bi2O3 collects holes from TiO2, leaving electrons free to react and increase by 5 times the photocatalytic efficiency toward H2 generation. This study provides new insight into the importance of the design and elaboration of optimal heterojunction based on the photocatalyst system to improve the photocatalytic activity.

关键词： photocatalysis     core-shell     heterojunction     H2     TiO2     Bi2O3    

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Rh<sub>2sub>O<sub>3sub>/hexagonal CePO<sub>4sub> nanocatalysts for N<sub>2sub>O decomposition

Huan Liu, Zhen Ma

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 586-593 doi: 10.1007/s11705-017-1659-6

摘要： Hexagonal CePO nanorods were prepared by a precipitation method and hexagonal CePO nanowires were prepared by hydrothermal synthesis at 150 °C. Rh(NO ) was then used as a precursor for the impregnation of Rh O onto these CePO materials. The Rh O supported on the CePO nanowires was much more active for the catalytic decomposition of N O than the Rh O supported on CePO nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO , O , H O or O /H O) on the N O decomposition was also investigated. The samples were characterized by N adsorption-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-programmed reduction, oxygen temperature-programmed desorption, and CO temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.

关键词： Rh2O3     CePO4     N2O decomposition    

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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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ZnFe<sub>2sub>O<sub>4sub> deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO<sub>2sub> 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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ZnFe<sub>2sub>O<sub>4sub>/BiVO<sub>4sub> Z-scheme heterojunction for efficient visible-light photocatalytic

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1728-1740 doi: 10.1007/s11705-023-2322-z

摘要： A novel Z-scheme ZnFe2O4/BiVO4 heterojunction photocatalyst was successfully synthesized using a convenient solvothermal method and applied in the visible light photocatalytic degradation of ciprofloxacin, which is a typical antibiotic contaminant in wastewater. The heterostructure of as-synthesized catalysts was confirmed using X-ray diffraction, scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectroscopy characterizations. Compared with the single-phase counterparts, ZnFe2O4/BiVO4 demonstrated considerably enhanced photogenerated charge separation efficiencies because of the Z-scheme transfer mechanism of electrons between the composite photocatalysts. Consequently, the 30% ZnFe2O4/BiVO4 catalyst afforded a degradation rate of up to 97% of 20 mg/L ciprofloxacin under 30 min of visible light irradiation with a total organic carbon removal rate of 50%, which is an excellent activity compared with ever reported BiVO4-based catalysts. In addition, the liquid chromatography-mass spectrometry and quantitative structure-activity relationships model analyses demonstrated that the toxicity of the intermediates was lower than that of the parent ciprofloxacin. Moreover, the as-synthesized ZnFe2O4/BiVO4 heterojunctions were quite stable and could be reused at least four times. This study thus provides a promising Z-scheme heterojunction photocatalyst for the efficient removal and detoxication of antibiotic pollutants from wastewater.

关键词： ZnFe2O4/BiVO4     Z-scheme heterojunction     photocatalytic degradation     ciprofloxacin    

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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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Tuning nitrogen defects and doping sulfur in carbon nitride for enhanced visible light photocatalytic

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 93-101 doi: 10.1007/s11705-022-2175-x

摘要： Defect construction and heteroatom doping are effective strategies for improving photocatalytic activity of carbon nitride (g-C3N4). In this work, N defects were successfully prepared via cold plasma. High-energy electrons generated by plasma can produce N defects and embed sulfur atoms into g-C3N4. The N defects obviously promoted photocatalytic degradation performance that was 7.5 times higher than that of pure g-C3N4. The concentration of N defects can be tuned by different power and time of plasma. With the increase in N defects, the photocatalytic activity showed a volcanic trend. The g-C3N4 with moderate concentration of N defects exhibited the highest photocatalytic activity. S-doped g-C3N4 exhibited 11.25 times higher photocatalytic activity than pure g-C3N4. It provided extra active sites for photocatalytic reaction and improved stability of N defects. The N vacancy-enriched and S-doped g-C3N4 are beneficial for widening absorption edge and improving the separation efficiency of electron and holes.

关键词： g-C3N4     nitrogen defect     sulfur doping     photodegradation     plasma    

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过硫酸盐诱导的缺陷氮化碳中三配位氮（N3<sub>Csub>）空位增强光催化产过氧化氢 Article

缪蔚, 王奕杰, 刘莹, 秦贺贺, 褚成成, 毛舜

《工程（英文）》 2023年 第25卷 第6期   页码 214-221 doi: 10.1016/j.eng.2021.12.016

摘要： 其中石墨氮化碳（g-C<sub>3sub>N<sub>4sub>）被认为是最有前途的合成过氧化氢的光催化剂之一；并且，在g-C<sub>3sub>N<sub>4sub>中引入氮空位已被证明是提高其光催化活性的有效策略在此，本文提出了一种简便的过硫酸钠共晶聚合方法，制备了具有丰富三配位氮空位（N3<sub>Csub>）的g-C<sub>3sub>N<sub>4sub>。本研究的结果表明，在g-C<sub>3sub>N<sub>4sub>中引入N3<sub>Csub>空位可以成功地拓宽光吸收范围，抑制光激发电荷的重组，增强O<sub>2sub>的吸附和活化富含N3<sub>Csub>空位的g-C<sub>3sub>N<sub>4sub>的光催化过氧化氢产量是原始g-C<sub>3sub>N<sub>4sub>的4.5倍。本研究提出了在g-C<sub>3sub>N<sub>4sub>中引入N3<sub>Csub>空位的新策略，为开发光催化产过氧化氢的活性催化剂提供了一种新方法。

关键词： 氮化碳     N3<sub>Csub>空位     过氧化氢     光催化     过硫酸盐    

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Highly effective visible-photocatalytic hydrogen evolution and simultaneous organic pollutant degradation

《环境科学与工程前沿（英文）》 2022年 第16卷 第10期 doi: 10.1007/s11783-022-1566-z

摘要：

● An urchin-like OMS/ZIS composite was fabricated by a facile solvothermal method.

关键词： Dual-functional photocatalysts     Oxygen-doped MoS2/ZnIn2S4     H2 evolution     Organic pollutant    

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Factors affecting photocatalytic performance through the evolution of the properties due to the phasetransition from NaBiO·2HO to BiO

《能源前沿（英文）》 2022年 第16卷 第3期   页码 471-482 doi: 10.1007/s11708-021-0778-4

摘要： The phase transition process of a photocatalytic system from NaBiO3·2H2O to BiO2–x has been investigated to understand the important factors that affect photocatalytic performance in a composite system. It is found that a proper amount of BiO2–x on the surface of NaBiO3·2H2O could effectively suppress the electron/hole recombination and increase the exposed reactive sites for photocatalytic reaction. A fully covered BiO2–x on NaBiO3·2H2O results in a dramatical decrease of photocatalytic degradation of dye. An over long hydrothermal process can result in BiO2–x with reduced oxygen vacancies, which degrades the photocatalytic activity. Furthermore, the photocatalytic reduction ability of CO2 conversion has been investigated, indicating that the surface activity to different reactants also directly affects the catalytic performance. The investigation of the gradient phase transition process presents a clear guidance to construct a desired photocatalytic system, in addition to selecting gradient materials with suitable bandgap structure and a morphology with different fraction and distribution of each component. The defect evolution of each component during construction of a composite is also an important factor that should be optimized and considered in making a composite to achieve high photocatalytic efficiency.

关键词： composite construction     distribution     BiO2–x     evolution of defects    

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标题 作者 时间 类型 操作

Decoration of CdMoO micron polyhedron with Pt nanoparticle and their enhanced photocatalytic performancein N fixation and water purification

期刊论文

Cu-doped Bi/Bi<sub>2sub>WO<sub>6sub> catalysts for efficient N<sub>2sub> fixation by photocatalysis

期刊论文

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

期刊论文

Cyanobacterial photo-driven mixotrophic metabolism and its advantages for biosynthesis

Ni Wan,Mary Abernathy,Joseph Kuo-Hsiang Tang,Yinjie J. Tang,Le You

期刊论文

In-MOF-derived In<sub>2sub>S<sub>3sub>/Bi<sub>2sub>S<sub>3sub> heterojunction for enhanced photocatalytic

期刊论文

Interfacial charge transfer and photocatalytic activity in a reverse designed BiO/TiO core-shell

期刊论文

Rh<sub>2sub>O<sub>3sub>/hexagonal CePO<sub>4sub> nanocatalysts for N<sub>2sub>O decomposition

Huan Liu, Zhen Ma

期刊论文

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

期刊论文

ZnFe<sub>2sub>O<sub>4sub> deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO<sub>2sub> in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

期刊论文

ZnFe<sub>2sub>O<sub>4sub>/BiVO<sub>4sub> Z-scheme heterojunction for efficient visible-light photocatalytic

期刊论文

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

期刊论文

Tuning nitrogen defects and doping sulfur in carbon nitride for enhanced visible light photocatalytic

期刊论文

过硫酸盐诱导的缺陷氮化碳中三配位氮（N3<sub>Csub>）空位增强光催化产过氧化氢

缪蔚, 王奕杰, 刘莹, 秦贺贺, 褚成成, 毛舜

期刊论文

Highly effective visible-photocatalytic hydrogen evolution and simultaneous organic pollutant degradation

期刊论文

Factors affecting photocatalytic performance through the evolution of the properties due to the phasetransition from NaBiO·2HO to BiO

期刊论文