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JOURNAL OF ALLOYS AND COMPOUNDS · 2019 · IF 4.175

Facile synthesis of three-dimensional WO3-x/Bi/BiOCl hierarchical heterostructures with broad spectrum driven photocatalytic activity

Yunfang Huang,Hui Xu,Dan Luo,Yuezhu Zhao,Yu Fang,Qiyao Guo,Yuelin Wei,Leqing Fan,Jihuai Wu

To improve the utilization efficiency of solar energy and separation of photogenerated carries, a novel three-dimensional (3D) WO 3-x /Bi/BiOCl hierarchical heterostructures with broad spectrum responsive photocatalytic activity have been fabricated through a facile solvothermal technique. The influences of varying loading of WO 3-x on the physical performances of the as-obtained composites were systematically characterized by X-ray diffraction, scanning electron microscope, transmission electron microscopy , X-ray photoelectron spectroscopy, optical absorbance, photoluminescence and specific surface areas. The WO 3-x /Bi/BiOCl displayed a strong optical absorption from 250 to 2500 nm, and showed the superior photocatalytic performance in degradation of rhodamine B (RhB) than that of individual components. Among the as-prepared samples, the sample S24 with the appropriate content of WO 3-x displayed the best photocatalytic performance, which can photodegrade RhB with the efficiency of 100%, 100% and 96% under the UV light within 8 min, visible light within 3 min and near-infrared light within 120 min exposure, respectively. Furthermore, a plausible mechanism of the RhB degradation on WO 3-x /Bi/BiOCl photocatalysts under the near-infrared light irradiation was proposed according to the photocatalytic activity and radical species trapping experiments.

研究领域: 材料科学 · 环境科学
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ACS Earth and Space Chemistry · 2024 · IF 2.9

Oxychlorine and Carbonate Generation by Simulated Electrostatic Discharge of Martian Dust Activities and Detection by Raman Spectroscopy

Junqi Ren,Wenshuo Mao,Zhongchen Wu,Xiaohui Fu,Qiyuan Hou,Mingyu Chen,Ziwei Fu

The Martian atmosphere and surface materials can be impacted by electrochemical reactions that occur during dust activity on Mars. Prior research has shown that in the dry Martian surface environment, electrostatic discharge (ESD) can generate oxychlorine along with converting CO2 to carbonate dust. To comprehend the carbon and chlorine cycles on Mars, research on carbonates and oxychlorine is crucial, as is investigating the effects of coexisting minerals. In support of this work, precise methods for measuring ESD reactions are needed. Herein, ESD reactions on chloride (NaCl) and potential coexisting minerals SiO2 or TiO2 were investigated under simulated Martian atmosphere conditions, and Raman spectroscopy was used to measure trace products. Based on Raman measurements, the influences of coexisting minerals on the production of carbonates and oxychlorine during ESD reactions were investigated. Our findings suggest that Raman spectroscopy has sensitive quantitative detection capabilities in aqueous solutions, offering a useful technique for the quantitative detection of laboratory products. Carbonate continuously accumulated with increasing discharge time, with 14–22 times greater yield (1.43–4.77‰ and 5% error) than perchlorate (0.10–0.24‰ and 20% error) and 5–16 times greater yield than chlorate (0.28–0.44‰ and 20% error). The yields of the above products were found to depend on the type, content, and particle size of coexisting minerals. Our findings are crucial for understanding the current geological history, atmospheric evolution, and substance cycling on Mars, as well as for retracing the development of Martian atmospheric and hydrological environments.

研究领域: 行星科学 · 地质学 · 化学
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CATALYSIS COMMUNICATIONS · 2015 · IF 3.699

Thermocatalytic deterioration of polymeric films with heat-sensitive S/BiOCl catalyst through naturally ambient-temperature excitation

Feng Ding,Sizhao Zhang,Xuegang Luo,Xiaoyan Lin

A novel S/BiOCl thermocatalyst in response to heat excitation was successfully synthesized by a one-step method and then added into polymeric matrix to give corresponding films. The results obtained show that the surfaces of as-prepared films with S/BiOCl were truly degraded via thermocatalytic reactions at ambient conditions. The average molecular weights of experimental films have fallen dramatically, comparing to the comparisons. In addition, the changes of chemical groups were simultaneously observed in the process. Thus this thermocatalytic process maybe a very fascinating route to come true the degradation of polymeric films with lower temperature triggered.

研究领域: 材料科学 · 高分子化学 · 环境功能材料 · 催化化学 · 纳米材料
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CHEMICAL PAPERS · 2020 ·Vol. 74 ·期 11 ·3987-3993 · IF 1.68

Determination and application of the reaction between REOCl (RE = Y, Gd and Sm) and H2O

Pan Binfeng,Zhang Zhimin,Lu Xuchen

Abstract The reaction between rare earth oxychloride (REOCl) and water was investigated. X-ray diffractometer, volumetric titrations, FTIR spectrograph and scanning electron microscope were used to determine the reaction process and the reaction products. It was found that the reaction could be concluded as follows: 5REOCl(s) + 5H 2 O(l) = 2RE 2 (OH) 5 Cl(s) + RE 3+ (aq) + 3Cl − (aq). Based on this reaction, a new method for determining the purity of anhydrous rare earth chloride was proposed. Compared with the conventional method, the maximum absolute error decreased from 22 to < 1% and the maximum relative error decreased from 111 to < 4% under the experimental conditions. Graphic abstract

研究领域: 化学 · 材料科学
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ACS Applied Energy Materials · 2024 · IF 5.4

In Situ Structural Self-Optimization and Oxygen Vacancy Creation to Boost the Stability of Bi-MOF Derived Bi2O3@C and BiOCl@C Anodes

Yanting Ma,Yan Tang,Yajuan Xu,Suisui Su,Shuzhen Chen,Shizheng Zheng,Changyuan Hu,Xin Li,Kejie Dai,Rongbin Zhang

Metal oxides are promising alkaline battery electrodes with high theoretical capacity, but the low energy density and poor stability make them far away from actual application. Herein, single Bi-MOF derived ultrastable Bi2O3@C and BiOCl@C anodes are architected via a two-for-one manner. Specifically, optimal Bi2O3@C anode with hierarchical and porous structure delivers high specific capacity (278.3 mAh g–1 at 1 A g–1) owing to the exposed electrochemical active sites, fast charge transfer, and efficient ion diffusion. More importantly, ultrahigh stability (110%, 5000 cycles) is achieved due to the in situ morphological self-optimization and oxygen vacancy creation. Similarly, BiOCl@C anode also displays remarkable capacity and ultralong cycling stability (94%, 15000 cycles) due to the conductive and protective carbon layer, abundant reactive centers, and ion transport channels. Moreover, the in situ phase transition of BiOCl to Bi2O2CO3 also contributes to the outstanding stability. Our work provides rational guidance for architecting high capacitive and ultrastable anodes for aqueous rechargeable alkaline battery.

CAS / MDL: 554-95-0
研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

In situ enhanced chlorine oxide radical generation on a novel space-confined photoanode and its application for ammonia oxidation: Structure, performance, and mechanism

Ting Su,Yunhe Gong,Xue Cui,Xinhong Wang,Yanan Zhang,Hongbin Yu

Oxidizing ammonia to nitrogen is a challenge in wastewater treatment. For this challenge ammonia oxidation via chlorine oxide radicals has been proved to be a potential method. In this study, a space-confined photoanode was designed and prepared by loading RuO 2 nanoparticles on TiO 2 /WO 3 nanowires for in situ enhancing the generation of chlorine oxide radical. Scanning electron microscopy characterization confirmed that RuO 2 nanoparticles were uniformly deposited on TiO 2 /WO 3 nanowires. The generation of chlorine oxide radical was markedly boosted, and its steady-state concentration reached 2.76 × 10 −12 M. This value was 3 times that of the traditional bifacial electrode (a type of electrode that has been widely used for chlorine oxide radical-related research). As a result, ammonia oxidation was greatly enhanced. In 90 min, 31.9 mg/L ammonia nitrogen could be degraded, yet only 0.94 mg/L nitrate was accumulated. In addition, the space-confined photoanode exhibited good performance for real wastewater treatment, and 41.0 mg/L ammonia nitrogen could be oxidized in 135 min. During photoelectrocatalysis, a synergistic index (47.7 %) was obtained. Besides the synergistic effect between photocatalysis and electrocatalysis, the unique morphology and structural design (TiO 2 /WO 3 and RuO 2 were mainly responsible to hydroxyl radical generation and free chlorine production, respectively) also synergistically promoted the generation of chlorine oxide radical, thereby improving ammonia oxidation. The mechanism for ammonia oxidation via chlorine oxide radicals over the space-confined photoanode was proposed based on experimental results and theoretical calculations.

CAS / MDL: 108-78-1 11140-77-5
研究领域: 环境科学 · 材料科学
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ELECTROCHIMICA ACTA · 2024 · IF 5.5

Chlorine-oxidation-free dual hydrogen production by seawater electrolysis coupling formaldehyde oxidation

Qi Wang,Xiangjian Liu,Jiawei Zhu,Heqing Jiang

The main challenges hindering the practical application of seawater electrolysis are the substantial energy input for sluggish oxygen evolution reaction (OER) and anode corrosion by chlorine oxidation reaction (COR). Here we report a simple but reliable strategy of coupling seawater electrolysis with formaldehyde oxidation reaction (FOR) to achieve energy-saving and COR-free dual hydrogen production . For the anode FOR, the onset potential is cut to near -0.2 V vs. the reversible hydrogen electrode (RHE) much lower than the theoretical potential of OER (1.23 V vs. RHE), and the Faradaic efficiencies of both hydrogen and high-value formate products achieve nearly 100 %. In a two-electrode electrolyzer at 100 mA cm −2 , the cell voltage of our integrated system is 1.75 V lower than that of the conventional seawater electrolysis, leading to a 66 % reduction in electricity consumption. Moreover, benefiting from the ultra-low reaction potential, the harmful COR is fundamentally avoided. This work opens up a new way to efficiently and stably convert sea resources into hydrogen fuel while also achieving chemical upgrades.

研究领域: 能源科学 · 电化学工程 · 可再生能源
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CHEMICAL ENGINEERING JOURNAL · 2016 · IF 5.31

Light-emitting diodes as an emerging UV source for UV/chlorine oxidation: Carbamazepine degradation and toxicity changes

Wen-Long Wang,Qian-Yuan Wu,Zhi-Ming Li,Yun Lu,Ye Du,Ting Wang,Nan Huang,Hong-Ying Hu

Carbamazepine (CBZ) is a ubiquitous micropollutant in wastewater and reclaimed water. In this study, we evaluated CBZ degradation by light-emitting diode (LED)-driven UV/chlorine oxidation. Under LED irradiation of 280   nm (LED280) and 310   nm (LED310), UV/chlorine could efficiently degrade CBZ. Compared with LED UV/H 2 O 2 treatment, LED UV/chlorine oxidation achieved a CBZ degradation rate that was one order of magnitude higher. The CBZ degradation followed pseudo-first-order kinetics, and the rate constants ( k obs,CBZ ) for LED280 UV/chlorine and LED310 UV/chlorine increased from 0.072 to 0.91   min −1 and 0.044 to 0.65   min −1 , respectively, when chlorine dosage increased from 0.07 to 0.14   mM. Under neutral conditions, the generated OH and Cl accounted for over 80% of the CBZ degraded by LED UV/chlorine. The maximum k obs,CBZ for LED UV/chlorine was observed at pH 8.5; k obs,CBZ decreased when solution pH increased to 9.5 or decreased to 5.5. This is because the main UV-absorbing chlorine species in the LED280 and LED310 systems is OCl − , which is different from those in low-pressure mercury lamp/chlorine systems. The acute toxicity for CBZ solution treated by LED UV/chlorine increased at lower fluence (<752   mJ/cm 2 ) and decreased at higher fluence (>1233   mJ/cm 2 ). However, the cytotoxicity to Chinese hamster ovary cells and adsorbable organic halide content of CBZ solution both increased after chlorination and LED UV/chlorine. The lowest electrical cost for the degradation of CBZ by LED UV/chlorine occurred under neutral conditions with a chlorine dosage of 0.4–0.7   mM (28.4–49.7   mg/L).

CAS / MDL: 64-18-6 98-95-3 75-65-0
研究领域: 环境科学 · 水处理技术 · 毒理学
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ORGANIC ELECTRONICS · 2017 · IF 3.399

TiO2/SnOxCly double layer for highly efficient planar perovskite solar cells

Cuncun Wu,Ziru Huang,Yihao He,Wei Luo,Hungkit Ting,Tieyi Li,Weihai Sun,Qiaohui Zhang,Zhijian Chen,Lixin Xiao

Recently, perovskite solar cells have attracted tremendous research interest due to their amazing light to electric power conversion efficiency (PCE). However, most high performance devices usually use mesoporous TiO 2 as the electron transport layer (ETL), which increases cost for practical application. Here, TiO 2 /SnO x Cl y double layer was employed as the ETL for planar perovskite solar cells . Compared with bare TiO 2 , perovskite solar cell based on TiO 2 /SnO x Cl y shows drastically improved power conversion efficiency and reduced hysteresis. These improvements are attributed to TiO 2 /SnO x Cl y which could enhance electron extraction and reduce surface trap-state.

研究领域: 材料科学 · 能源技术
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Catalysts · 2025 ·Vol. 15 ·期 4 ·382 · IF 4

Geometric Matching Effect Induced High Dispersion of Na2WO4 Nanocluster on Cristobalite Support for Efficient Methyl Chloride-to-Vinyl Chloride Conversion

Nan Lu,Yifeng Shi,Yutao Ren,Yue Wang,Xinyi Sun,Zejing Wei,Xutao Chen,Jie Fan

The oxidative coupling of methyl chloride (CH3Cl) to vinyl chloride (C2H3Cl) (MCTV) represents a promising yet challenging direct conversion route for C2H3Cl production. In this study, a novel catalyst, cristobalite silica, supported Na2WO4nanoclusters, was fabricated by calcining an intermediate composite composed by β-zeolite and sodium tungstate (Na2WO4). The pore structure of this β-zeolite possesses a regular shape and suitable size distribution, providing an accurate geometric matching effect for Na2WO4to homogeneously distribute in the entire β-zeolite matrix with high loading. Accordingly, the excellent dispersity of Na2WO4nanocluster active sites is well maintained even after calcining at 750 °C, and the microporous β-zeolite matrix is completely converted to dense cristobalite phase silica after the calcination. The high-loading and well-dispersed Na2WO4nanocluster leads to a superior performance in MCTV with a CH3Cl conversion of 81.5%, a C2H3Cl selectivity of 42.4%, and a C2H3Cl yield of 34.6%. Notably, the catalyst exhibits remarkable stability during the catalytic process.

CAS / MDL: 9003-11-6
研究领域: 化学工程 · 催化材料科学
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Environmental Science-Water Research & Technology · 2022 ·Vol. 8 ·期 11 ·2744-2760 · IF 5.819

Experimental study and quantum chemical calculation of free radical reactions in ciprofloxacin degradation during the UV/chlorine oxidation process

Ziru Li,Xia Yuan,Huili Tang,Xu Jiang,Chunge Wu,Lu Zheng,Erdeng Du,Mingguo Peng

The UV/chlorine process was utilized to degrade a common quinolone, ciprofloxacin, in water. Ciprofloxacin removal was high at 92.2% in 100 s, with a first-order rate constant of 0.0026 s−1 during the process. The degradation of ciprofloxacin was found to be positively related to UV intensity and chlorine dosage and negatively related to ammonia concentration. According to FMO, MSPA, CDFT, and topological quantum chemical analysis, the N6 or N7 atoms are the most vulnerable to electrophilic or radical attacks in the piperazine ring ciprofloxacin structure, indicating the most likely reactive sites for the initial reaction. 21 degradation products were identified, including 19 products by HRMS LC–MS and 2 by GC–MS. These intermediates were mainly produced through the following three pathways: the piperazine ring's cleavage, hydroxyl addition, and defluorination reaction. Both the acute toxicity tests and ECOSAR prediction illustrated that the ecological risks cannot be effectively removed due to the production of more toxic intermediates during the degradation process.

研究领域: 环境科学 · 化学工程 · 药学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Polyoxometalate-loaded hyper-crosslinked nanoparticles as a Pickering interfacial catalyst for solvent-free epoxidation of allyl chloride under static conditions

Qianyu Zha,Jigang An,Bowen Jiang,Ying Liu,Zhongguang Zhang,Jia Liu,Zhibing Zhang

Epoxidation of allyl chloride and hydrogen peroxide (H 2 O 2 ) carried out in heterogeneous catalytic systems suffer from poor reaction efficiency due to their heavy mass transfer resistance present at the liquid-liquid interface. Pickering interfacial catalysis (PIC) provides an elegant solution by involving the design of amphiphilic heterogeneous catalysts , which can act as emulsifiers simultaneously. In this study, interface-active polyoxometalate-loaded hyper-crosslinked nanoparticles (HCNPs) were designed. The structural properties of materials were characterized in detail by elemental analysis , Zeta potential , ICP-OES, SEM , TEM, BET, FT-IR, TGA , and XPS . The prepared nanoparticles can build efficient W/O PIC systems with allyl chloride and H 2 O 2 . Systematic experiments indicate that catalysts' surface properties, catalyst dosage, and water/oil volume ratio significantly affect the PIC system's catalytic activity and emulsion properties. Moreover, this PIC system maintains high stability after the reaction and can be reused for at least 8 cycles. Excitingly, these interface-active HCNPs can also efficiently promote allyl chloride epoxidation in the absence of solvent and external stirring, illustrating that this approach holds great potential for developing catalytic systems suitable for multiphase reactions.

研究领域: 化学工程 · 材料科学 · 催化化学
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