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INORGANIC CHEMISTRY · 2019 · IF 4.85

Particulate Oxynitride Photoanodes Assembled with Transparent Electron-Collecting Oxide Nanorod Arrays

Feng-Qiang Xiong,Beibei Dong,Shuwen Yu

The collection of photogenerated electrons is commonly a bottleneck in photoelectrochemical water oxidation on a particulate photoanode. Herein, a new strategy called “array insertion” for particulate photoanode preparation is proposed to improve electron collection. ZnO nanorod arrays are inserted between LaTiO2N particles and Al-doped ZnO (AZO) substrates via epitaxial electrodeposition, which make electronic connections. Using this methodology, charge separation efficiency is improved drastically, and the photocurrent at 1.23 VRHE is enhanced by more than 1 order of magnitude, because the obstacle of electron collection in the particulate LaTiO2N photoanodes is overcome.

研究领域: 材料科学 · 电化学 · 能源转换
✓ 已验证 DOI 高影响因子
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ChemSusChem · 2019 ·Vol. 12 ·期 11 ·2480-2486 · IF 7.804

Metal–Organic Gel-Derived Multimetal Oxides as Effective Electrocatalysts for the Oxygen Evolution Reaction

Zhengmao Cao,Zhongwei Jiang,Yang Li,Chengzhi Huang,Yuanfang Li

Graphical Who let the MOGs out? This work reports a compositionally alterable metal–organic gel (MOG) to obtain spinel-type metal oxide (MO) with excellent electrocatalytic oxygen evolution reaction (OER) activity. The capacity for catalytic water oxidation could be improved by adjusting the metal composition and ratio in the MOG. This investigation provides a facile approach to obtain multimetal oxides with high electrocatalytic performance. Exploring efficient and durable catalysts derived from earth-abundant and cost-effective materials is a highly desirable route to overcome the sluggish anodic oxygen evolution reaction (OER). A series of multinary metal–organic gels (MOGs) with various and alterable metal element compositions are prepared by straightforward mixing of metal ions with ligand 4,4′,4′′-[(1,3,5-triazine-2,4,6-triyl)tris(azanediyl)]tribenzoic acid (H 3 TATAB) in solution at room temperature. Spinel-type metal oxides with excellent electrocatalytic OER performance were then obtained through calcination of the as-synthesized MOGs. In electrochemical testing, the trimetallic oxide CoFeNi-O-1 (derived from the MOG with a Co/Fe/Ni molar ratio of 5:1:4) exhibits remarkable catalytic activity with a low overpotential of 244 mV at a current density of 10 mA cm −2 and a small Tafel slope of 55.4 mV dec −1 in alkaline electrolyte, outperforming most recently reported electrocatalysts. This work not only provides a promising OER catalyst and enriches the application of MOGs in the catalytic field, but also offers a facile new route to acquiring multicomponent metal oxides with high electrocatalytic activity.

研究领域: 材料科学 · 电化学 · 催化科学
✓ 已验证 DOI PubMed 高影响因子
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FUEL · 2018 · IF 4.908

Iron based monolithic catalysts supported on Al2O3, SiO2, and TiO2: A comparison for NO reduction with propane

Hao Zhou,MengYao Ge,Shiguo Wu,Bichao Ye,Yaxin Su

The selective catalytic reduction of NO with propane has been investigated with iron based monolithic catalysts supported on alumina, silica, and titania. The catalysts were characterized by N 2 -physisorption, XRD, SEM, XPS, H 2 -TPR, Py-FTIR and in situ DRIFTS technologies. The different supports had a significant influence on specific surface area, surface morphology, lattice oxygen, redox properties and the acid sites, which resulted in differences in the catalytic activity of NO reduction. The C 3 H 8 -SCR performance decreased in the order as Fe/Al 2 O 3 /CM > Fe/SiO 2 /CM > Fe/TiO 2 /CM. Fe/Al 2 O 3 /CM showed the highest activity with a nitrogen oxide conversion of 100% in the presence of oxygen at 500 °C,which is mainly attributed to the good redox properties and the abundant Lewis acid sites. Based on in situ DRIFT studies, the increase of Lewis acid sites will enhance the formation of NO 2 /NO 3 − species and acetate/formate species, then promote the catalytic activity.

研究领域: 催化化学 · 环境科学
✓ 已验证 DOI 高影响因子
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JOURNAL OF MATERIALS SCIENCE · 2021 ·Vol. 56 ·期 16 ·10108-10123 · IF 4.22

Graphene oxide–cerium oxide hybrids for enhancement of mechanical properties and corrosion resistance of epoxy coatings

Ma Lingwei,Wang Xuanbo,Wang Jinke,Zhang Juantao,Yin Chengxian,Fan Lei,Zhang Dawei

In this study, graphene oxide–cerium oxide (GO–CeO 2 ) hybrids were synthesized through an in situ hydrothermal approach and were incorporated into epoxy resin to prepare a robust coating for aluminum alloy protection. The mechanical properties of the GO–CeO 2 -loaded coating were characterized by nano-indentation, friction-wear test and pull-off adhesion test, using pristine epoxy coating and GO-loaded epoxy coating for comparison. Results revealed that GO–CeO 2 addition could increase the hardness, elastic modulus and the wear resistance and decrease the friction coefficient of the composite coating. Compared with pristine epoxy coating, the adhesion strength of GO–CeO 2 /epoxy coating increased from 7.3 MPa to 12.2 MPa. Such improvement in the mechanical properties can be explained by the good dispersion of GO–CeO 2 in the composite coating. In addition, salt spray and electrochemical impedance spectroscopy (EIS) measurement results showed that the corrosion resistance of the GO–CeO 2 -loaded coating was significantly enhanced. After 30 days of salt spray test, the coating resistance of the GO–CeO 2 /epoxy coating was 17.8 and 3.5 times higher compared with that of the blank epoxy coating and GO/epoxy coating, respectively. The superior barrier performance of the composite coating was mainly ascribed to the synergistic effects of the prolonged pathway against corrosive media permeation and the corrosion inhibition effect of CeO 2 particles.

研究领域: 材料科学 · 表面工程 · 防腐蚀技术
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Journal of Water Process Engineering · 2019 · IF 3.173

Sulfamethoxazole removal enhancement from water in high-silica ZSM-5/ozonation synchronous system with low ozone consumption

Senlin Ma,Xingtao Zuo,Juan Xiong,Cong Ma,Zhongbing Chen

An ozonation process combined with hydrophobic adsorbent high silica ZSM-5 (HSZSM-5) was designed to enhance sulfamethoxazole (SMX) removal and reduce the ozone consumption. The promoted effect of HSZSM-5 on SMX removal was investigated in terms of SMX removal and TOC removal efficiency as well as the ozone consumption. The impacts of pH and CO 3 2− /HCO 3 - were also analyzed. The presence of HSZSM-5 helped to increase the SMX degradation and TOC removal efficiency and their kinetics rate constants. HSZSM-5 adsorption behaviors for SMX and its degradation intermediates were responsible for the findings. Direct ozone oxidation was the main mechanism of SMX removal as HZSM-5 could not contribute to producing H 2 O 2 and •OH. Much higher CO 3 2− /HCO 3 - concentration (≥10 mM) and pH value (>7) were in favor of SMX degradation. HSZSM-5 had a positive contribution to SMX removal. The mass ratio of ozone consumption to the removed SMX reduced to 0.63 g O 3 /g SMX. This system of introducing high silica zeolite in the ozonation/adsorption process is an environmentally and economically sound technology to removal micropollutants.

研究领域: 环境科学 · 水处理技术
✓ 已验证 DOI 高影响因子
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Reaction Chemistry & Engineering · 2021 ·Vol. 6 ·期 8 ·1475-1482 · IF 4.239

Hydrodeoxygenation of sulfoxides into sulfides under mild conditions over a heterogeneous cobalt catalyst

Yanxin Wang,Kaiyue Yao,Duanjian Tao,Nian Xiang,Wei Wang,Zehui Zhang

In this study, Al2O3/nitrogen-doped carbon supported cobalt catalysts (Co–NC/Al2O3-T, where T represents the pyrolysis temperature) were successfully prepared by a one-step pyrolysis method and studied for the hydrodeoxygenation of sulfoxides into sulfides. The structure of the Co–NC/Al2O3-T catalysts was greatly affected by the pyrolysis temperature, and thus the pyrolysis temperature showed a great influence on the catalytic activity of the Co–NC/Al2O3-T catalysts. The Co–NC/Al2O3-500 catalyst demonstrated excellent catalytic performance for the hydrodeoxygenation of sulfoxides into sulfides with yields from 94% to 98% under mild conditions (80 °C and 10 bar H2), and the catalytic activity of Co–NC/Al2O3-500 was found to be comparable with that of reported noble metal catalysts. Both the support and the metallic cobalt nanoparticles crucially contributed to the excellent catalytic activity of the Co–NC/Al2O3-500 catalyst. More importantly, the Co–NC/Al2O3-500 catalyst showed a good stability after five runs.

研究领域: 催化化学 · 材料科学
✓ 已验证 DOI 高影响因子
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Catalysts · 2022 ·Vol. 12 ·期 9 ·1034 · IF 4.501

Effect of Morphology-Dependent Oxygen Vacancies of CeO2 on the Catalytic Oxidation of Toluene

Ahmed Ismail,Muhammad Zahid,Boren Hu,Adnan Khan,Nauman Ali,Yujun Zhu

Catalytic oxidation is regarded as an effective, economical, and practical approach to remove volatile organic compounds such as important air pollutants. CeO2catalysts with different morphologies exhibit different oxygen vacancies content, which plays a vital role in oxidation reaction. Herein, three distinct morphologies of CeO2i.e., shuttle (CeO2(S)), nanorod (CeO2(R)), and nanoparticle (CeO2(P)), were successfully fabricated by the SEM and TEM results, and investigated for toluene catalytic oxidation. The various characterizations showed that the CeO2(S) catalyst exhibited a larger surface area along with higher surface oxygen vacancies in contrast to CeO2(R) and CeO2(P), which is responsible for its excellent toluene catalytic oxidation. The 90% toluene conversion temperature at 225 °C over CeO2(S) was less than that over CeO2(R) (283 °C) and CeO2(P) (360 °C). In addition, CeO2(S) showed a greater reaction rate (14.37 × 10−2μmol∙g−1∙s−1), TOFov(4.8 × 10−4∙s−1) at 190 °C and lower activation energy value (67.4 kJ/mol). Furthermore, the CeO2(S) also displayed good recyclability, long-term activity stability, and good tolerance to water. As a result, CeO2(S) is considered a good candidate to remove toluene.

研究领域: 环境科学 · 催化化学
✓ 已验证 DOI 高影响因子
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Green Synthesis and Catalysis · 2020 · IF 0

Enhanced activity for aerobic oxidative of alcohols over manganese oxides stimulated with interstitial nitrogen doping

Fei Ruan,Fengfeng Li,Zhengping Dong,Qingping Ke,Yangxin Jin,Wangcheng Zhan,Minh Ngoc Ha,Jun Tang

Heteroatom-doped transition-metal oxides are potential non-noble-metal-based catalysts for the aerobic oxidation of alcohols because of the synergistic effects of their multiple active sites. However, the design of efficient heteroatom-doped transition-metal oxide catalysts is hindered by the complexity of the synergistic effects of multiple active sites. We have developed a practical strategy for fabricating nitrogen-doped MnO 2 ( N –MnO 2 ), in which nitrogen is selectively doped at interstitial sites in MnO 2 . Use of N –MnO 2 as a catalyst enabled additive-free aerobic oxidation of alcohols in > 99% yield at 30 ​°C. The catalytic activity of commercial MnO 2 (< 1%) was negligible. Systematic studies of a series of Mn-based oxide catalysts, namely commercial MnO 2 , MnN x O 2− x (prepared by traditional N doping by treatment with NH 3 ), and N –MnO 2 showed that N –MnO 2 with abundant interstitial nitrogen dopant (1.8 ​mol%) had the best catalytic activity. Mechanistic studies suggested that the introduction of interstitial nitrogen as a dopant in MnO 2 enhanced the adsorption and dissociation of oxygen on the N –MnO 2 catalyst and promoted oxidative dehydrogenation of alcohols at interstitial nitrogen and oxygen vacancy sites. In situ infrared spectroscopy showed that C–N bonds (1161 ​cm −1 ) were formed and broken during benzyl alcohol oxidation. This confirms the importance of interstitial nitrogen in the catalytic cycle. This work provides an alternative strategy based on interstitial nitrogen doping for designing nitrogen-doped transition-metal oxides for aerobic oxidative reactions.

研究领域: 化学 · 材料科学
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Science China-Materials · 2015 ·Vol. 58 ·期 7 ·534-542 · IF 0

Rational design of graphene oxide and its hollow CoO composite for superior oxygen reduction reaction

Zhang Guoxin,Xu Yuqi,Wang Lin,Wang Jindi,Kuang Yun,Sun Xiaoming

Graphene oxide (GO) is an important derivative of graphene, fascinating the entire world with its dazzling properties and versatile performance. However, the synthesis of GO via chemical routes often results in limited control of the density of functionalities and their distribution, presenting a barrier to the spread of GO applications. We modified Hummers’ method and aimed at controlling the oxygen functionality of GO. The highest oxygen content of the modified synthetic GO (MdGO) occurs at edge regions, and the large proportion of carboxyl groups can be easily removed upon annealing. The excellent conductivity of intrinsic graphene can thus be recovered after the removal of the main functional groups. The resulting MdGO was reduced and doped with NH 3 , and the reduced MdGO (rMdGO) was determined to be an excellent support for oxygen reduction reaction (ORR) electrocatalysts. As a demonstration, a composite of CoO and N-rMdGO was fabricated, which exhibited highly comparable ORR performance in alkaline relative to 20 wt.% Pt/C.

研究领域: 材料科学 · 电化学
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ACS Sustainable Chemistry & Engineering · 2021 · IF 8.198

Peroxidase Mimicking of Binary Polyacrylonitrile-CuO Nanoflowers and the Application in Colorimetric Detection of H2O2 and Ascorbic Acid

Xuefang Zheng,Qi Lian,Liya Zhou,Yanjun Jiang,Jing Gao

A simple and efficient strategy was developed to synthesize polyacrylonitrile-copper oxide (PAN-CuO) nanoflowers by growing copper oxide nanoneedles on the surface of polyacrylonitrile (PAN) nanoflowers under mild conditions. Fortunately, the obtained PAN-CuO nanoflowers exhibit excellent peroxidase-mimicking activity to catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to form a blue-colored solution with H2O2. The peroxidase-like mechanism originated from the generation of the •OH radical. The PAN-CuO-based colorimetric assay was used to detect H2O2 with a detection limit (LOD) of 0.12 μM in a linear range from 0.5 to 125 μM. The colorimetric method was simple, selective, and sensitive for ascorbic acid (AA) detection in the range of 1–180 μM with a detection limit (LOD) of 0.56 μM. Moreover, the proposed PAN-CuO-based colorimetric assay could be used in the real sample analysis. The peroxidase-like PAN-CuO nanoflowers could provide a versatile catalytic platform for the application of the colorimetric assay method and biomimetic enzyme catalytic systems, and open a new way for detection of AA in biological systems.

研究领域: 材料科学 · 生物化学 · 分析化学
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Fabrication of metal oxides-based adsorbents for SO2 capture with equimolar adsorption

Yuqi Yang,Xiandong Hao,Zhongxiao Sun,Yuan Chen,Zhiyong Xu,Wenbo Zhao

A series of novel porous metal oxides (MO, M = Mg, Ca, Ba, Mn and Zn) adsorbents were synthesized through simple thermal treatment of the corresponding metal sulfite for the remotion of sulfur dioxide (SO 2 ). The obtained MO adsorbents were characterized by various techniques including scanning electron microscopy (SEM), thermal gravimetric analyzer (TGA), X-ray diffraction (XRD) and nitrogen adsorption studies. The results show that the SO 2 adsorption capacity of manganese oxide (MnO) is much higher than that of other MO. And due to its highly dispersed and large specific surface area, especially its well-developed pore structure, equimolar adsorption of SO 2 can be achieved for the first time among similar SO 2 adsorbents. In addition, different sources of MnO were explored and it was found that the MnO obtained from the decomposition of MnSO 3 had the highest SO 2 adsorption capacity. Adsorption kinetic studies show that the reaction between MnO and SO 2 conforms to the pseudo-second-order kinetic equation. Furthermore, it was found through seven-cycle experiments that the adsorption amount tended to stabilize in each of the following cycles, except for the first high temperature, which led to changes in the adsorbent and a decrease in cycling performance. This strategy has three advantages: one-step preparation at low temperatures, equimolar adsorption of SO 2 as well as good reusability and selectivity.

研究领域: 环境科学 · 材料科学
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Oxygen nanobubbles enhanced photodegradation of oxytetracycline under visible light: Synergistic effect and mechanism

Lei Wang,Jafar Ali,Zhibin Wang,N.A. Oladoja,Rong Cheng,Changbo Zhang,Gilles Mailhot,Gang Pan

Nanobubbles have gained much attention due to their unusual properties such as large specific surface area, surface energy and internal energy, thereby, increase the surface reaction and improve the mass transfer efficiency. The long term stability of nanobubbles and generation of reactive oxygen species enables them to address various environmental issues for water purification without secondary pollution. However, there are few studies concerning the application of oxygen nanobubbles in the advanced oxidation processes (AOPs). In this study, first time, oxygen nanobubbles were introduced into the photoreaction system under visible light irradiation for enhanced photodegradation of oxytetracycline (OTC). Results indicated that oxygen nanobubbles significantly improved the photodegradation of OTC through high mass transfer and generation of reactive radicals during the nanobubble collapse. The oxygen nanobubble stability was confirmed to be pH dependent. The nanobubbles concentration increased from 0.76 to 3.78 × 10 8  particles/mL, while the mean size decreased from 205 nm to 138 nm as the pH value increased (3.2–11.0). The photodegradation efficiency of OTC was improved from 45% to 98% with the increase of pH (4.0–11.0). Oxygen nanobubbles hold promise to improve the AOPs , such as reducing catalysts and chemicals usage and costs. Quenching experiments demonstrated that OH was the predominant active species induced the photodegradation of OTC. With the development of nanobubbles technology, it is anticipated to realize totally chemicals free green technology. This study provides a novel nanobubble/AOPs technology, which will be more efficient and environmental friendly and will have broad application in waste water treatment and drinking water purification.

研究领域: 环境科学 · 化学工程
✓ 已验证 DOI 高影响因子
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