Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 10
·5430-5441
·
IF 14.511
Huaijie Shi,Ge Feng,Suiqin Li,Jia Liu,Xinying Yang,Ye Li,Ye Lu,Xing Zhong,Shibin Wang,Jianguo Wang
An alternative method for producing ozone, electrochemical ozone production (EOP) is a major area of interest in the field of in situ sterilization and disinfection. However, commercial lead dioxide as a traditional anodic electrocatalyst is highly toxic and has low durability, and exploring anodic electrocatalysts with lower lead content and performance loss is challenging. Herein, a series of pyramidal sillenite-type Bi12PbO20 materials were designed and fabricated with a hydrothermal method in which Pb was introduced to Bi2O3 frameworks. The product, Bi12PbO20-3, exhibited remarkable EOP performance, with faradaic efficiency of 15.1% at 50 mA cm−2 in a neutral solution, which was almost 1.5 times that of commercial β-PbO2. Computational simulations further demonstrated that the confined [Pb–O4] fragment was confined in the Bi–O bonding environment of Bi12PbO20, the low oxygen vacancy formation energy resulted from the weak Pb–O interaction and remarkably enhanced EOP activity. Such a local confined environment plays a vital role in suppressing Pb loss, thereby accounting for the robust EOP stability. Additionally, the significant performance of the membrane electrode assembly system in the electrochemical degradation of antibiotics and pesticides implied the potential environmental application capabilities of Bi12PbO20.
研究领域:
材料科学
·
环境科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Qinghe Liu,Sen Wang,Fei Han,Shupei Lv,Zairong Yan,Yunfei Xi,Jing Ouyang
Highly efficient three-dimensional (3D) kaolinite/MnO2–CuO (KM@CuO–NO3) catalysts were synthesized by a mild biomimetic strategy. Kaolinite flakes were uniformly wrapped by ultrathin tremelliform MnO2 nanosheets with thicknesses of around 1.0–1.5 nm. Si–O and Al–O groups in kaolinite hosted MnO2 nanosheets to generate a robust composite structure. The ultrathin MnO2 lamellar structure exhibited excellent stability even after calcination above 350 °C. Kaolinite/MnO2 exhibited abundant edges, sharp corners, and interconnected diffusion channels, which are superior to the common stacked structure. Open channels guaranteed fast transportation and migration of CO and O2 during CO oxidation. The synthesized KM@CuO–NO3 achieved a 90% CO conversion efficiency at a relatively low temperature (110 °C). Furthermore, the abundant oxygen vacancies on KM@CuO-NO3 assisted the adsorption and activation of oxygen species and thus enhanced the oxygen mobility and reactivity in the catalytic process. The mechanism results suggest that CuO introduced to the catalyst not only acted as CO active sites but also weakened the Mn–O bond, subsequently improved the mobilities of the oxygen species, which was found to contribute to its high activity for CO oxidation. This study provides new conceptual insights into rationally regulating structural assembly between transition metal oxides and natural minerals for high-performance catalysis reactions.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Shaoyu Tang,Lei Xu,Xiaolong Yu,Shuona Chen,Huanyong Li,Ying Huang,Junfeng Niu
Degradation of capecitabine was conducted using electrochemical oxidation, UV/H 2 O 2 oxidation, and ozonation. Capecitabine was efficiently degraded by three advanced oxidation processes. The degradation rates of capecitabine achieved approximately 99.0% after 4 min of ozonation, 12 min of electrochemical oxidation, and 30 min of UV/H 2 O 2 oxidation. The mineralization rate obtained was merely 10.3% for ozonation at 60 min, compared to 91.7% for electrochemical oxidation and 55.3% for UV/H 2 O 2 oxidation. Capecitabine was degraded by oxidation, defluorination, hydrogenation, hydrolysis, ring and bond cleavage. Thus, multiple intermediates were generated during the degradation process, such as F - , formic acid, acetic acid, oxalic acid, and other intermediate metabolites with lager molecules. A total of eighteen metabolites, except for F - and carboxylic acids, were identified by QTOF-HRMS, where six of them could only be detected by the electrochemical oxidation process, two of them were by the UV/H 2 O 2 oxidation process, and one of them by the ozonation process. Electrochemical oxidation was the only process that could achieve over 90% removal of cytotoxicity and genotoxicity, and the metabolites were non-genotoxic after 60 min of reaction. The number of live cells decreased with the increasing reaction time in ozonation, demonstrating the higher toxicity of the intermediates in ozonation. Energy cost evaluation results suggested that the lowest energy consumption was achieved at 1.8 kWh/m 3 for 90% of capecitabine degradation with the O 3 dosage of 250 mg/h. Energy consumptions for 50% removal of cytotoxicity were 21.3 and 6.3 kWh/m 3 in electrochemical oxidation and UV/H 2 O 2 oxidation, respectively. The highest energy cost for 50% of genotoxicity removal was observed in electrochemical oxidation, while ozonation was identified as the most cost-effective process.
研究领域:
环境科学
·
化学工程
·
药学
·
毒理学
✓ 已验证
产品关联
DOI
高影响因子
JACS Au
·
2023
·
IF 8
Yizhou Yang,Jili Li,Chong Li,Ming Gong,Xue Wang,Xuejing Yang,Hualin Wang,Ye-Fei Li,Zhi-Pan Liu
Nickel peroxides are a class of stoichiometric oxidants that can selectively oxidize various organic compounds, but their molecular level structure remained elusive until now. Herein, we utilized structural prediction using the Stochastic Surface Walking method based on a neural network potential energy surface and advanced characterization using the as-synthesized nickel peroxide to unravel its chemical identity as the bridging superoxide containing nickel hydroxide, or nickel superoxyhydroxide. Superoxide incorporation tunes the local chemical environment of nickel and oxygen beyond the conventional Bode plot, offering a 6.4-fold increase in the electrocatalytic activity of urea oxidation. A volcanic dependence of the activity on the oxygen equivalents leads to the proposed active site of the Ni(OO)(OH)Ni five-membered ring. This work not only unveils the possible structures of nickel peroxides but also emphasizes the significance of tailoring the oxygen environment for advanced catalysis.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 75
·47435-47447
·
IF 3.108
Donglin He,Huiping Zhang,Ying Yan
CuO over ZSM-5 zeolite membrane was prepared by chemical vapor deposition (CVD) for catalytic wet peroxide oxidation (CWPO) of phenol in a fixed bed reactor. Firstly, Cu-ZSM-5/PSSFs catalysts with Cu loading of 2 wt%, 4 wt% and 6 wt% were prepared and characterized by XRD, XPS, SEM, EDS, N2 adsorption–desorption and TPR (H2), respectively. Compared with CuO deposited directly onto PSSFs, the CuO supported on ZSM-5/PSSFs tended to be more regular with smaller crystal size. Then, several parameters affecting H2O2 consumption and phenol oxidation such as reaction temperature, Cu loading, and different supports were investigated in the CWPO of phenol with a high concentration (1 g L−1 phenol and 5.1 g L−1 H2O2). Experimental results revealed that Cu-ZSM-5/PSSFs (6%) showed better activity for the oxidation of phenol than Cu-ZSM-5/PSSFs catalysts with lower Cu loading and CuO/PSSFs with same theoretical loading. A complete reduction of phenol and a high TOC removal around 60% had been achieved over Cu-ZSM-5/PSSFs (6%) at the temperature of 80 °C, feed flow rate of 2 mL min−1 and catalyst bed height of 2 cm. Finally, the possible oxidation pathway of phenol was studied based on the by-products detected by high-performance liquid chromatography (HPLC).
研究领域:
环境科学
·
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 3
·1524-1530
·
IF 3.361
Fan Bai,Lincheng Xu,Daode Wang,Li An,Zhanzhong Hao,Fan Li
Manganese oxide composites with mixed valence states were prepared through the hydrothermal method by compositing with Ti4O7 and calcining at different temperatures, and their ORR and OER catalytic performance were investigated. The prepared catalysts were characterized by XRD, SEM-EDS, HRTEM-EDS, and XPS methods to analyse their phase constitution, morphology feature, and surface composition. The major phase of manganese oxides was Mn3O4, which is a one-dimensional structure, and its growth was induced by Ti4O7. The ORR and OER catalytic activity can be enhanced due to the preferred orientation of manganese oxides. Electrochemical measurements, namely CV, LSV and EIS, were utilized for determining the ORR and OER catalytic activity, whereas CA and ADT were used for studying the durability and stability. A Li–O2 battery was assembled to test the electrochemical behavior and properties in practical application. MnOx/Ti4O7 calcined at 300 °C exhibited the best catalytic activity of 0.72 V vs. RHE half-wave potential for ORR and 0.67 V vs. RHE overpotential for OER. The proportion of Mn3+ was also highest in all the MnOx/Ti4O7 composites. The assembled Li–O2 battery shows high performance with a voltage gap of only 0.85 V. Therefore, it can be affirmed that the inducement of Ti4O7 could strengthen the preferred orientation in manganese oxide growth and Mn3+ in MnOx/Ti4O7 plays a vital role in catalyzing ORR and OER, with both improving the ORR and OER bifunctional catalytic performance of manganese oxides.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yi Fang,Shoubing Chai,Zhiwei Chu,Zirui He,Yingjie Li
In the calcium looping CO 2 capture process, using CO in the flue gas to reduce NO at a high molar ratio of CO to NO (e.g., above 10:1) can achieve efficient removal of NO. However, the lots of unreacted CO causes secondary pollution. In this study, a novel Cu/Ce co-modified CaO was proposed for cyclic CO 2 capture and the catalytic NO reduction at a low CO:NO molar ratio (e.g., 2:1). The experimental findings indicate that Cu/Ce modification improves the performance of CaO in both catalytic NO reduction and carbonation. The Cu/Ce co-modified CaO contained the optimal Cu/Ce/Ca molar ratio of 1:5:100 possesses both NO removal and CO conversion efficiencies of above 99 %, along with CO 2 removal efficiency exceeding 88%. Microscopic analysis determines that the electron transfer between Cu and Ce facilitates the conversion of lattice oxygen into surface oxygen, mitigating the competition between CO 2 and CO for surface oxygen. Furthermore, density functional theory calculations demonstrate that CO/NO/CO 2 exhibits non-competitive adsorption behavior on Cu/Ce co-modified CaO. Consequently, Cu/Ce-modified CaO possesses superior catalysis for efficient NO reduction by CO at low CO:NO molar ratio in calcium looping process.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Shiqi Peng,Rong Li,Yu Huang,Yufei Zhang,Jun-ji Cao,Shuncheng Lee
Producing the strong metal-support interaction (SMSI) interface and highly reactive oxygen species is a great challenge for catalytic oxidation of formaldehyde (HCHO) at room temperature over supported metal catalysts. Herein, we report a conceptual oxygen vacancy ( V O ) associated SMSI interface of Pt-ZrO 2 nanoparticles for HCHO catalysis at room temperature, exhibiting interfacial dependent reactive oxygen species (O*) formation. The V O on the ZrO 2 support captures and activates the molecular O 2 , then proceeds to generating the reactive oxygen atom (O*) with a lower activation barrier of 0.3 eV. The generated O* tends to link the (1 1 0) surface of ZrO 2 and the (1 1 1) surface of Pt as an electronic transmission channel for the selective catalytic oxidation of HCHO adsorbed on the (1 1 0) surface of ZrO 2 , accelerating the direct generation of formate species and mineralization of HCHO. The Pt- V O -ZrO 2 achieves high HCHO removal and HCHO conversion (>95%) at 20 °C. These findings will consolidate the fundamental theories of room temperature catalytic reactions via constructing the SMSI interface engineering for wide environmental applications.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 26
·13150-13159
·
IF 11.301
Huan Liu,Xiaoning Li,Cailing Peng,Liuyang Zhu,Yuanxi Zhang,Huiru Cheng,Jiameng Cui,Qingmei Wu,Yingying Zhang,Zezhi Chen,Wei Zou,Wen Gu,Haoliang Huang,Jianlin Wang,Bangjiao Ye,Zhengping Fu,Yalin Lu
The catalytic activity for the oxygen evolution reaction (OER) in electrocatalytic water splitting strongly depends on the adsorption energy of intermediates. For the generally proposed adsorbate evolution route, the universal scaling relation between the adsorption energies of *OOH and *OH leads to an OER efficiency limitation based on the “volcano curve”. A possible solution to bypass the scaling relation is to avoid the formation of the *OOH intermediate in the OER with the participation of lattice oxygen from catalysts. In this work, the lattice oxygen in (Bi0.5Co0.5)2O3 is activated through adjusting the Fermi energy level and the strong overlap between Co 3d and O 2p, by means of increasing the oxygen vacancy concentration. Compared to oxygen-vacancy-poor (Bi0.5Co0.5)2O3, the oxygen-vacancy-rich (Bi0.5Co0.5)2O3 exhibits a significantly lower Tafel slope (43 mV dec−1), 15 times higher mass activity, 18 times higher turnover frequency, and excellent long-term stability in alkaline media, superior to those of the benchmark OER electrocatalyst IrO2. This work provides a feasible strategy to activate lattice oxygen with fast OER kinetics and puts forward the development of efficient and stable catalysts towards water oxidation.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 39
·18476-18484
·
IF 3.3
Bin Liu,Haoliang Ruan,Chengyi Li,Jie Yao,Bei Wei,Lei Wang,Shurong Ban,Jun Xie
In this work, InCex nanoparticles with different In–Ce ratios were synthesized by a simple co-precipitation method and InCex nanoparticles could be used as a mimic of peroxidase to catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) by H2O2 and produce the typical blue ox TMB. In addition, the prepared InCex nanoparticles showed excellent peroxidase-like catalytic properties compared with pure CeO2 and pure In2O3. InCe0.1 exhibited the best peroxidase-like activity, which was mainly attributed to the indium–cerium synergy, which accelerated the TMB and H2O2 electron transfer rate between them. Based on the above findings, a facile and sensitive H2O2 detection system with a sensitive response range of 10–100 μM and a detection limit of 5 μM for H2O2 was successfully proposed. This work synthesizes nanomaterials with peroxidase-like activity by modifying In2O3 through a simple co-precipitation method and offers new insights into the search for novel peroxidase mimics.
研究领域:
生物化学
·
材料科学
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Research and Technology-JMR&T
·
2023
·
IF 6.4
Yun-Yang Li,Hao-Jie Yan,Lian-Kui Wu,Fa-He Cao
To improve the high temperature oxidation resistance of TiAl alloy, silicon oxycarbide (SiOC) coating was fabricated by dip-coating using polydimethylsiloxane (PDMS) as the precursor. The oxidation behavior of the coating was evaluated at 850 °C. The morphology and chemical structure of the SiOC coating were characterized by scanning electron microscopy (SEM) equipped with an energy dispersive spectroscopy (EDS), Fourier Transform infrared spectroscopy (FT-IR), X-ray photo electron spectroscopy (XPS), and X-ray diffraction (XRD). Results showed that the SiOC coating exhibited good oxidation resistance. During the thermal exposure, the selective oxidation of Al at the SiOC/TiAl alloy interface resulted in the generation of protective Al 2 O 3 , which suppressed the inward diffusion of oxygen and outward diffusion of the alloy matrix elements. However, the cracks on the surface of SiOC coating were observed, which would provide channels for the oxygen and form thermally grown oxide layer (mainly consisting of TiO 2 and Al 2 O 3 ) above the Al 2 O 3 layer.
研究领域:
材料科学
·
表面工程
✓ 已验证
产品关联
DOI
高影响因子
ENERGY
·
2017
·
IF 4.52
J. Yan,C.Y. Zhao,Z.H. Pan
Cyclic stability is a key factor in the design of thermochemical heat storage systems . Because carbon dioxide (CO 2 ) may react with heat storage materials and lead to a decrease in energy storage efficiency, the effect of CO 2 on Ca(OH) 2 /CaO and Mg(OH) 2 /MgO systems is investigated in this study. The experimental results show that CO 2 reacts with CaO in the water vapor that appears during the heat release process. Therefore, in the design of Ca(OH) 2 /CaO systems, CO 2 should be cleared from the system. The results from Mg(OH) 2 /MgO systems show that CO 2 only slightly reacts with MgO and Mg(OH) 2 during heat storage and release processes. This study indicates that carbonic acid (H 2 CO 3 ) could easily react with CaO/Ca(OH) 2 to form CaCO 3 during heat release processes. Generally, the remaining CO 2 reduces the reversibility of Ca(OH) 2 /CaO systems but has only a slight influence on Mg(OH) 2 /MgO systems. In addition, the experimental results show that carbonate shell does not exist in rehydration for both of the CaO/MgO samples, but the influence of CO 2 on the entire process increases after each cycle.
研究领域:
材料科学
·
能源工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）