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Cu-doped Bi/Bi2sub>WO6sub> catalysts for efficient N2sub> 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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Fabrication of highly efficient Bi

Wei Mao, Lixun Zhang, Tianye Wang, Yichen Bai, Yuntao Guan

《环境科学与工程前沿（英文）》 2021年第15卷第4期 doi: 10.1007/s11783-020-1344-8

摘要： Abstract • A novel Bi2WO6/CuS composite was fabricated by a facile solvothermal method. • This composite efficiently removed organic pollutants and Cr(VI) by photocatalysis. • The DOM could promoted synchronous removal of organic pollutants and Cr(VI). • This composite could be applied at a wide pH range in photocatalytic reactions. • Possible photocatalytic mechanisms of organic pollutants and Cr(VI) were proposed. A visible-light-driven Bi2WO6/CuS p-n heterojunction was fabricated using an easy solvothermal method. The Bi2WO6/CuS exhibited high photocatalytic activity in a mixed system containing rhodamine B (RhB), tetracycline hydrochloride (TCH), and Cr (VI) under natural conditions. Approximately 98.8% of the RhB (10 mg/L), 87.6% of the TCH (10 mg/L) and 95.1% of the Cr(VI) (15 mg/L) were simultaneously removed from a mixed solution within 105 min. The removal efficiencies of TCH and Cr(VI) increased by 12.9% and 20.4%, respectively, in the mixed solution, compared with the single solutions. This is mainly ascribed to the simultaneous consumption electrons and holes, which increases the amount of excited electrons/holes and enhances the separation efficiency of photogenerated electrons and holes. Bi2WO6/CuS can be applied over a wide pH range (2–6) with strong photocatalytic activity for RhB, TCH and Cr(VI). Coexisiting dissolved organic matter in the solution significantly promoted the removal of TCH (from 74.7% to 87.2%) and Cr(VI) (from 75.7% to 99.9%) because it accelerated the separation of electrons and holes by consuming holes as an electron acceptor. Removal mechanisms of RhB, TCH, and Cr(VI) were proposed, Bi2WO6/CuS was formed into a p-n heterojunction to efficiently separate and transfer photoelectrons and holes so as to drive photocatalytic reactions. Specifically, when reducing pollutants (e.g., TCH) and oxidizing pollutants (e.g., Cr(VI)) coexist in wastewater, the p-n heterojunction in Bi2WO6/CuS acts as a “bridge” to shorten the electron transport and thus simultaneously increase the removal efficiencies of both types of pollutants.

关键词： Photocatalysis Bi₂WO₆/CuS Organic pollutants Cr(VI) Synergistic effect

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Morphology selective construction of

Maher Darwish, Ali Mohammadi, Navid Assi, Samer Abuzerr, Youssef Alahmad

《化学科学与工程前沿（英文）》 2020年第14卷第4期页码 561-578 doi: 10.1007/s11705-019-1808-1

摘要： Controlled growth of Bi WO nanorods with exposed [0 0 1] facets and the fabrication of an Fe O -Bi WO magnetic composite by a microwave-assisted polyol process, were achieved in this study. The adsorptivity and photocatalytic performance of the composite toward sunset yellow dye degradation were greatly enhanced by the -cyclodextrin cavities on its surface, firmly anchored through a cetyltrimethylammonium bromide linkage. A series of examinations and characterizations were carried out to determine the influence of various factors on the morphological modulation-photocatalytic behavior of the pure Bi WO prior to final functionalization. Changing the pH of the precursor solution impacted the formation of 0D, 2D, and 3D structures; however, the presence of hexamethylenetetramine surfactant induced the development of 1D nanorod structure. A reasonable crystal growth mechanism was proposed to elucidate the formation process. Conversely, the mechanism of the activity enhancement of -cyclodextrin functionalized Fe O -Bi WO , compared to that of the non-functionalized samples, could be realized with the assistance of chemical trapping experiments on sunset yellow, and was confirmed on the colorless antibiotic (sulfamethoxazole). The high performance and durability of this composite can be attributed to the facet-dependent activity, large adsorption capacity due to inclusion interactions, enhanced visible light absorption, and efficient charge separation.

关键词： β-cyclodextrin Bi₂WO₆ shape controlled nanorod sunset yellow

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Effective degradation of tetracycline by mesoporous Bi

Xiaolong CHU,Guoqiang SHAN,Chun CHANG,Yu FU,Longfei YUE,Lingyan ZHU

《环境科学与工程前沿（英文）》 2016年第10卷第2期页码 211-218 doi: 10.1007/s11783-014-0753-y

摘要： Bi WO was synthesized with a hydrothermal method at different pHs and used for the degradation of tetracycline (TC) in water. The mesoporous Bi WO prepared at pH 1 (BWO-1) displayed the highest adsorption and degradation capacity to TC due to its large surface area and more efficient capacity to separate photogenerated electrons and holes. 97% of TC at 20 mg·L was removed by BWO-1 at 0.5 g·L after 120 min irradiation under simulated solar light. Only 31% of the total organic carbon (TOC) was removed after 360 min irradiation although the TC removal reached 100%, suggesting that TC was mainly transformed to intermediate products rather than completely mineralized. The intermediates were identified by high-performance liquid chromatography-time of flight-mass spectrometry (HPLC-TOF-MS) and possible photodegradation pathways were proposed.

关键词： Bi₂WO₆ hydrothermal synthesis tetracycline (TC) photocatalysis

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Piezocatalytic performance of FeO−BiMoO catalyst for dye degradation

《化学科学与工程前沿（英文）》 2023年第17卷第6期页码 716-725 doi: 10.1007/s11705-022-2265-9

摘要： A Fe₂O₃−Bi₂MoO₆ heterojunction was synthesized via a hydrothermal method. Scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray, powder X-ray diffraction, Fourier transform infrared spectroscopy and ultra-violet−visible near-infrared spectrometry were performed to measure the structures, morphologies and optical properties of the as-prepared samples. The various factors that affected the piezocatalytic property of composite catalyst were studied. The highest rhodamine B degradation rate of 96.6% was attained on the 3% Fe₂O₃−Bi₂MoO₆ composite catalyst under 60 min of ultrasonic vibration. The good piezocatalytic activity was ascribed to the formation of a hierarchical flower-shaped microsphere structure and the heterostructure between Fe₂O₃ and Bi₂MoO₆, which effectively separated the ultrasound-induced electron–hole pairs and suppressed their recombination. Furthermore, a potential piezoelectric catalytic dye degradation mechanism of the Fe₂O₃−Bi₂MoO₆ catalyst was proposed based on the band potential and quenching effect of radical scavengers. The results demonstrated the potential of using Fe₂O₃−Bi₂MoO₆ nanocomposites in piezocatalytic applications.

关键词： piezocatalysis Fe₂O₃−Bi₂MoO₆ dye decomposition ultrasonic vibration

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Photoreduction adjusted surface oxygen vacancy of BiMoO for boosting photocatalytic redox performance

《化学科学与工程前沿（英文）》 2023年第17卷第12期页码 1937-1948 doi: 10.1007/s11705-023-2353-5

摘要： In this study, Bi₂MoO₆ with adjustable rich oxygen vacancies was prepared by a novel and simple solvothermal-photoreduction method which might be suitable for a large-scale production. The experiment results show that Bi₂MoO₆ with rich oxygen vacancies is an excellent photocatalyst. The photocatalytic ability of BMO-10 is 0.3 and 3.5 times higher than that of the pristine Bi₂MoO₆ for Rhodamine B degradation and Cr(VI) reduction, respectively. The results display that the band energy of the samples with oxygen vacancies was narrowed and the light absorption was broadened. Meanwhile, the efficiency of photogenerated electron-holes was increased and the separation and transfer speed of photogenerated carriers were improved. Therefore, this work provides a convenient and efficient method to prepare potential adjustable oxygen vacancy based photocatalysts to eliminate the pollution of dyes and Cr(VI) in water.

关键词： Bi₂MoO₆ oxygen vacancies photoreduction Cr(VI) RhB

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Photoelectrocatalytic generation of H and S from toxic HS by using a novel BiOI/WO nanoflake array photoanode

《能源前沿（英文）》 2021年第15卷第3期页码 744-751 doi: 10.1007/s11708-021-0775-7

摘要： In this paper, a photoelectrocatalytic (PEC) recovery of toxic H₂S into H₂ and S system was proposed using a novel bismuth oxyiodide (BiOI)/ tungsten trioxide (WO₃) nano-flake arrays (NFA) photoanode. The BiOI/WO₃ NFA with a vertically aligned nanostructure were uniformly prepared on the conductive substrate via transformation of tungstate following an impregnating hydroxylation of BiI₃. Compared to pure WO₃ NFA, the BiOI/WO₃ NFA promotes a significant increase of photocurrent by 200%. Owing to the excellent stability and photoactivity of the BiOI/WO₃ NFA photoanode and I^–/

I 3 −

catalytic system, the PEC system toward splitting of H₂S totally converted S^2– into S without any polysulfide (

S x n −

) under solar-light irradiation. Moreover, H₂ was simultaneously generated at a rate of about 0.867 mL/(h·cm). The proposed PEC H₂S splitting system provides an efficient and sustainable route to recover H₂ and S.

关键词： bismuth oxyiodide (BiOI)/ tungsten trioxide (WO₃) nano-flake arrays (NFA) photoelectrocatalytic (PEC) H₂S splitting H₂ S

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All-inorganic TiO/CsAgBiBr composite as highly efficient photocatalyst under visible light irradiation

《化学科学与工程前沿（英文）》 2023年第17卷第12期页码 1925-1936 doi: 10.1007/s11705-023-2344-6

摘要： In recent years, limited photocatalysis efficiency and wide band gap have hindered the application of TiO₂ in the field of photocatalysis. A leading star in photocatalysis has been revealed as lead-free Cs₂AgBiBr₆ double halide perovskite nanocrystals, owing to its strong visible light absorption and tunable band gap. In this work, this photocatalytic process was facilitated by a unique TiO₂/Cs₂AgBiBr₆ composite, which was identified as an S-cheme heterojunction. TiO₂/Cs₂AgBiBr₆ composite was investigated for its structure and photocatalytic behavior. The results showed that when the perovskite dosage is 40%, the photocatalytic rate of TiO₂ could be boosted to 0.1369 min^–1. This paper discusses and proposes the band gap matching, carrier separation, and photocatalytic mechanism of TiO₂/Cs₂AgBiBr₆ composites, which will facilitate the generation of new ideas for improving TiO₂’s photocatalytic performance.

关键词： Cs₂AgBiBr₆ nanocrystals visible-light photocatalyst Cs₂AgBiBr₆/TiO₂ heterojunction

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In-MOF-derived In2sub>S3sub>/Bi2sub>S3sub> 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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Chemical deactivation of V

Xiaodong WU, Wenchao YU, Zhichun SI, Duan WENG

《环境科学与工程前沿（英文）》 2013年第7卷第3期页码 420-427 doi: 10.1007/s11783-013-0489-0

摘要： V O -WO /TiO catalyst was poisoned by impregnation with NH Cl, KOH and KCl solution, respectively. The catalysts were characterized by X-ray diffraction (XRD), inductively coupled plasma (ICP), N physisorption, Raman, UV-vis, NH adsorption, temperature-programmed reduction of hydrogen (H -TPR), temperature-programmed oxidation of ammonia (NH -TPO) and selective catalytic reduction of NO with ammonia (NH -SCR). The deactivation effects of poisoning agents follow the sequence of KCl>KOH>>NH Cl. The addition of ammonia chloride enlarges the pore size of the titania support, and promotes the formation of highly dispersed V=O vanadyl which improves the oxidation of ammonia and the high-temperature SCR activity. K ions are suggested to interact with vanadium and tungsten species chemically, resulting in a poor redox property of catalyst. More importantly, potassium can reduce the Br?nsted acidity of catalysts and decrease the stability of Br?nsted acid sites significantly. The more severe deactivation of the KCl-treated catalyst can be mainly ascribed to the higher amount of potassium resided on catalyst.

关键词： V₂O₅-WO₃/TiO₂ potassium chloride poisoning reducibility acid sites

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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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Effective regeneration of thermally deactivated commercial V-W-Ti catalysts

Xuesong SHANG, Jianrong LI, Xiaowei YU, Jinsheng CHEN, Chi HE

《化学科学与工程前沿（英文）》 2012年第6卷第1期页码 38-46 doi: 10.1007/s11705-011-1167-z

摘要： An effective method for the regeneration of thermally deactivated commercial monolith SCR catalysts was investigated. Two types of regenerated solutions, namely NH Cl (1 mol/L) and dilute H SO (0.5 mol/L), were employed to treat the used catalyst. The effects of temperature and the regeneration process on the structural and textural properties of the catalysts were determined by X-ray diffraction, scanning electron microscopy, N adsorption/desorption, elemental analysis and Fourier transform infrared spectroscopy. The results suggest that the anatase phase of the used catalyst is maintained after exposure to high temperatures. Some of the catalytic activity was restored after regeneration. The catalyst regenerated by aqueous NH Cl had a higher activity than that of the catalyst treated by dilute H SO . The main reason is that the NH generated from the decomposition of NH Cl at high temperatures can be adsorbed onto the catalyst which promotes the reaction. The aggregated V O were partially re-dispersed during the regeneration process, and the intrinsic oxidation of ammonia with high concentrations of O is a factor that suppresses the catalytic activity.

关键词： V₂O₅-WO₃/TiO₂ catalysts thermal deactivation regeneration NH₄Cl dilute H₂SO₄ solution

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Review on cryogenic technologies for CO removal from natural gas

Yujing BI, Yonglin JU

《能源前沿（英文）》 2022年第16卷第5期页码 793-811 doi: 10.1007/s11708-022-0821-0

摘要： CO₂ in natural gas (NG) is prone to condense directly from gas to solid or solidify from liquid to solid at low temperatures due to its high triple point and boiling temperature, which can cause a block of equipment. Meanwhile, CO₂ will also affect the calorific value of NG. Based on the above reasons, CO₂ must be removed during the NG liquefaction process. Compared with conventional methods, cryogenic technologies for CO₂ removal from NG have attracted wide attention due to their non-polluting and low-cost advantages. Its integration with NG liquefaction can make rational use of the cold energy and realize the purification of NG and the production of by-product liquid CO₂. In this paper, the phase behavior of the CH₄-CO₂ binary mixture is summarized, which provides a basis for the process design of cryogenic CO₂ removal from NG. Then, the detailed techniques of design and optimization for cryogenic CO₂ removal in recent years are summarized, including the gas-liquid phase change technique and the gas-solid phase change technique. Finally, several improvements for further development of the cryogenic CO₂ removal process are proposed. The removal process in combination with the phase change and the traditional techniques with renewable energy will be the broad prospect for future development.

关键词： cryogenic CO₂ removal purification of natural gas (NG) biogas upgrading CH₄-CO₂ binary system

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Rh2sub>O3sub>/hexagonal CePO4sub> nanocatalysts for N2sub>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