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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    

Cu-doped Bi/Bi2WO6 catalysts for efficient N2 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    

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    

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    

A mini review on chemical fixation of CO 2 : Absorption and catalytic conversion into cyclic carbonates

Weili DAI, Chaktong AU, Shenglian LUO, Shuangfeng YIN,

《化学科学与工程前沿(英文)》 2010年 第4卷 第2期   页码 163-171 doi: 10.1007/s11705-009-0235-0

摘要: In this article, we present our research results on chemical fixation of CO using organobismuth compounds. We fabricated bismuth biphenoate complex, Zn-Mg-Al composite oxides, and SBA-15 or Al-SBA-15 immobilized hydroxyl ionic liquid for CO cycloaddition onto epoxides. The hypervalent bismuth compounds show good ability for association and dissociation with CO. The bismuth biphenolate complexes are catalytically effective for the cycloaddition reaction. The heterogeneous catalysts, viz. Zn-Mg-Al oxides and SBA-15 or Al-SBA-15 immobilized ionic liquid, are efficient for the synthesis of cyclic carbonate from CO and epoxide. It is found that the presence of a trace amount of water can improve the catalytic activity of the immobilized ionic liquid.

关键词: SBA-15     CO cycloaddition     Al-SBA-15 immobilized     CO     dissociation    

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    

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    

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    

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    

Plasmonic Au nanoparticles supported on both sides of TiO2 hollow spheres for maximising photocatalytic

Jianwei Lu, Lan Lan, Xiaoteng Terence Liu, Na Wang, Xiaolei Fan

《化学科学与工程前沿(英文)》 2019年 第13卷 第4期   页码 665-671 doi: 10.1007/s11705-019-1815-2

摘要: A strategy of intensifying the visible light harvesting ability of anatase TiO hollow spheres (HSs) was developed, in which both sides of TiO HSs were utilised for stabilising Au nanoparticles (NPs) through the sacrificial templating method and convex surface-induced confinement. The composite structure of single Au NP yolk-TiO shell-Au NPs, denoted as Au@Au(TiO , was rendered and confirmed by the transmission electron microscopy analysis. Au@Au(TiO showed enhanced photocatalytic activity in the degradation of methylene blue and phenol in aqueous phase under visible light surpassing that of other reference materials such as Au(TiO by 77% and Au@P25 by 52%, respectively, in phenol degradation.

关键词: TiO2 hollow spheres     plasmonic Au nanoparticles     confinement     visible light     photocatalytic degradation    

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    

Facile synthesis and enhanced visible-light photocatalytic activity of Ti

Xiaojie Zhang,Lei Wang,Shuqing Chen,Yi Huang,Zhuonan Song,Miao Yu

《化学科学与工程前沿(英文)》 2015年 第9卷 第3期   页码 349-358 doi: 10.1007/s11705-015-1523-5

摘要: Ti -doped TiO nanosheets with tunable phase composition (doped TiO (A/R)) were synthesized via a hydrothermal method with high surface area anatase TiO nanosheets TiO (A) as a substrate, structure directing agent, and inhibitor; the activity was evaluated using a probe reaction-photocatalytic CO conversion to methane under visible light irradiation with H as an electron donor and hydrogen source. High-resolution transmission electron microscope (HRTEM), field emission scanning electron microscope, UV-Vis diffuse reflectance spectra, and X-ray diffraction (XRD) etc., were used to characterize the photocatalysts. XRD and HRTEM measurements confirmed the existence of anatase-rutile phase junction, while Ti and single-electron-trapped oxygen vacancy in the doped TiO (A/R) photocatalyst were revealed byelectron paramagnetic resonance (EPR) measurements. Effects of hydrothermal synthesis temperature and the amount of added anatase TiO on the photocatalytic activity were elucidated. Significantly enhanced photocatalytic activity of doped TiO (A/R) was observed; under the optimized synthesis conditions, CH generation rate of doped TiO (A/R) was 2.3 times that of Ti -doped rutile TiO .

关键词: Ti3+-doped TiO2     photocatalytic CO2 conversion     visible light irradiation    

In-MOF-derived In2S3/Bi2S3 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    

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    

过硫酸盐诱导的缺陷氮化碳中三配位氮(N3C)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-C3N4)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-C3N4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(N3C)的g-C3N4。本研究的结果表明,在g-C3N4中引入N3C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O2的吸附和活化富含N3C空位的g-C3N4的光催化过氧化氢产量是原始g-C3N4的4.5倍。本研究提出了在g-C3N4中引入N3C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     N3C空位     过氧化氢     光催化     过硫酸盐    

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/Bi2WO6 catalysts for efficient N2 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

A mini review on chemical fixation of CO 2 : Absorption and catalytic conversion into cyclic carbonates

Weili DAI, Chaktong AU, Shenglian LUO, Shuangfeng YIN,

期刊论文

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

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

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

期刊论文

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

期刊论文

Plasmonic Au nanoparticles supported on both sides of TiO2 hollow spheres for maximising photocatalytic

Jianwei Lu, Lan Lan, Xiaoteng Terence Liu, Na Wang, Xiaolei Fan

期刊论文

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

期刊论文

Facile synthesis and enhanced visible-light photocatalytic activity of Ti

Xiaojie Zhang,Lei Wang,Shuqing Chen,Yi Huang,Zhuonan Song,Miao Yu

期刊论文

In-MOF-derived In2S3/Bi2S3 heterojunction for enhanced photocatalytic

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

过硫酸盐诱导的缺陷氮化碳中三配位氮(N3C)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