ACS Catalysis
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2023
·
IF 12.9
Yanfei Liu,Zhang Liu,Chengxiong Wang,Jie Xu,Jianping Ai,Xiao Liu,Aimin Zhang,Yunkun Zhao,Chun Du,Bin Shan
Supported Pt catalysts suffer from low reaction selectivity (<65% at 100% conversion) in the selective catalytic oxidation of ammonia (NH3-SCO) because of their intrinsic over-oxidation tendencies. Herein, a strategy based on facilitating byproduct NOx reduction to N2 is demonstrated at CuOx/PtCu catalysts, aiming to tackle the low selectivity challenge. This PtCu alloy sample with a CuOx-rich surface displays an N2 selectivity of 95%, while its turnover frequencies are the highest among reported supported Pt-based catalysts. The enhanced reaction activities and N2 selectivities are primarily attributed to the Pt-Cuδ+ dual-site synergies at the CuOx/PtCu interface, in which dual sites exhibit distinct NH3 adsorption, activation, and dehydrogenation behaviors. The Olat assisted internal selective catalytic reduction mechanism at CuOx/PtCu with N2O22– as the central intermediates is proposed. Density functional theory calculation and temperature-programmed surface reaction measurements show that the N–O bond in N2O22– tends to break simultaneously with the assistance of Ov in CuOx followed by the easy transition from N2O22– to N2, which serve as the origin of the high selectivity.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Hengyang Mao,Hengqi Shi,Zhijie Zhang,Shouyong Zhou,Minghui Qiu,Mingmin Jia,Meisheng Li,Yijiang Zhao,Shanshan Xia,Zhentao Wu
Ceramic membranes have drawn attention in oil-in-water (O/W) treatment due to natural hydrophilicity and excellent chemical stability, however their application was restricted by high cost. In this work, a cost-effective Al 2 O 3 -based ceramic support was prepared at sintering temperature of 1500 °C with low-cost mixed-dimensional attapulgite (MDATP) as aid. The composite support with addition of 10 wt% MDATP and 3 wt% powdered carbon possessed an average pore size of 3 µm, bending strength of 63.7 MPa, pure water permeability of 1.32 × 10 4 L·m −2 ·h −1 ·bar −1 . Mullite was formed due to the reaction between Al 2 O 3 and SiO 2 in MDATP during sintering, which played a key role in preparing support with corrosive resistance performance. Then, a superwetting microfiltration (MF) membrane with pore size of 0.18 µm and permeability of 1470 L·m −2 ·h −1 ·bar −1 was obtained by coating ATP nanofiber on the Al 2 O 3 -MDATP support with sintering temperature of 600 °C. The molecular dynamics results showed that the ATP can repel oil fouling with interaction energy of − 872 Kcal·mol −1 . The excellent O/W emulsion separation efficiency of the MF membrane further demonstrated the feasibility of ATP and its by-products in decreasing membrane cost and improving performance.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Yayu Guan,Jiaying Yan,Yuyu Liu,Fanghua Ning,Jin Yi,Jiujun Zhang
Electrochemical CO 2 reduction reaction (eCO 2 RR) is considered an efficient approach to produce value-added chemicals and fuels. In this paper, a series of MOF-derived composite catalysts with coexisting In 2 O 3 and ZnO are fabricated using a simple process for eCO 2 RR to produce formate. The Zn-In-O/800 catalyst achieves a formate Faradaic efficiency (FE HCOO− ) of 94.25 % at −1.16 V vs. RHE, which can maintain over 89 % after 30 h in a stability test. The electrochemical evidence and density functional theory analysis show that the strong interface effect between In 2 O 3 and ZnO can enhance the CO 2 adsorption and activation, and promote the conversion of CO 2 to formate. In addition, the ZnO phase can protect In 2 O 3 , as the main active site, from being reduced to a certain extent for a long time under negative potential, which ensures the high stability of the composite catalyst.
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WOOD SCIENCE AND TECHNOLOGY
·
2023
·Vol. 57
·期 4
·879-901
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IF 3.4
Luo Lingcong,Zhang Qianqian,Lan Yuling,Deng Jianping,Lin Yang,Du Guanben,Zhao Weigang
High-performance electrodes of activated carbons (PNOACs) with P, N, and O heteroatoms were prepared through a simple one-step phosphoric acid activation method without the need for any dopants or post-treatment. In the preparation procedure, cork biomass material from Quercus variabilis was used as the precursor, and phosphoric acid was used as both the phosphoric resource and the activation agent. The pore structure, morphology, and physicochemical properties of the as-prepared carbons were investigated. In addition, the electrochemical performances of the PNOACs were evaluated using three-electrode and two-electrode systems (symmetric supercapacitor, AS). The results indicated that cork is promising as a low-cost and environmental-friendly precursor for producing high-performance supercapacitors electrode. Furthermore, galvanostatic charge–discharge analysis revealed a specific capacitance of 206 F g −1 at a current density of 0.5 A g −1 , which can be attributed to the excellent hierarchical pore structure (micro-, meso-, and macropores) and suitable pore size distribution of the PNOACs. The specific surface area and total pore volume as high as 515.80 m 2 g −1 and 0.29 cm 3 g −1 were obtained, respectively. The presence of heteroatoms, namely N (0.81–1.07%), P (0.52–2.06%), and O (15.87–19.18%) content, on the carbon surface resulted in a considerable enhancement in the capacitive performance. Furthermore, a PNOAC sample, prepared at 600 °C with a mass ratio of 1:1, exhibited high long-term cycling stability (84.5%) and an energy density of 15.03 W h kg −1 . Therefore, cork is highly promising as an electrode material for supercapacitors to attain exceptional electrochemical performance, as well as provide a new possibility for the utilization and valorization of high-value cork waste.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Jili Yuan,Hao Yin,Xin Ge,Ronglan Pan,Caijuan Huang,Dechao Chen,Lin Hu,Haibo Xie
The coordination environment of transition metals in single-atom catalysts (SACs) is crucial for tuning the pathway of the electrocatalytic oxygen reduction reaction (ORR). However, it is significantly difficult to simultaneously and precisely control the first and second coordination structure near the metal active center. Herein, we report that the activated carbon black was used to anchor transition metals’ single atoms with a similar first and second coordination structure. As a result, Co-SACs exhibit an extraordinary performance for ORR to produce H 2 O 2 , where a current density of around ∼2.8 mA cm −2 at 0.1 V vs RHE by rotating ring-disk electrodes and a high yield rate of 110.2 mmol g metal −1 h −1 at the potential of 0.3 V vs RHE in a gas diffusion electrodes (GDEs) cell, with a high positive onset potential of 0.65 V vs RHE and a >80% selectivity of H 2 O 2 at the potential range from 0.25 to 0.65 V vs RHE, respectively. The combined experimental observations and theoretical calculations indicate that the catalytic active center lies in the Co-C 3 /O 1 moiety of the adjacent epoxy group. The possible position of the epoxy group in the second coordination sphere was further revealed. Moreover, Co-SACs were employed in an electrocatalytic GDEs cell for distributed generation of H 2 O 2 in the acidic media, and coupling Fe-SACs-based Fenton filter or electro-Fenton setup with the H 2 O 2 electrolytic generator delivers an efficient and distributable wastewater treatment system. Our study provides a promising and alternative route for on-site H 2 O 2 production coupling the practical application process.
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FOOD HYDROCOLLOIDS
·
2022
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IF 11.504
Yilan Wu,Yan Li,Bin Li,Yangyang Zhang,Yuehan Wu,Shilin Liu
In this study, the effect of bacterial cellulose nanofibrils (BCNF) surface charge density on the emulsification capacity of gelatin (GLT)/BCNF mixtures was investigated. Emulsions with 50 v% oil phase were co-stabilized by GLT and BCNFs (surface charge densities varied from 0.34 to 1.16 mmol/g) at pH 7.0 (GLT and BCNFs were negatively charged) and pH 4.7 (electrostatic equilibrium point for all GLT/BCNF mixtures). At pH 7.0, as BCNF surface charge density increased, the oil-water interfacial tension was decreased. Thus, the emulsion droplet size was reduced from 14.24 to 13.51 μm when the BCNF surface charge density was improved from 0.34 to 1.16 mmol/g. Additionally, the emulsion stability was significantly improved by the addition of highly-charged BCNF due to the increased electrostatic repulsion between dispersed droplets. At pH 4.7, the highest level of attractive electrostatic interaction was observed for GLT and BCNF with a surface charge density of 1.16 mmol/g (BCNF 1.16). Thus, the GLT/BCNF 1.16 suspension exhibited the highest viscoelastic modulus. At pH 4.7, the stability of GLT/BCNFs co-stabilized emulsions was improved by increasing BCNF surface charge density due to the enhanced viscosity. The emulsions prepared with GLT and BCNFs with surface charge density higher than 0.66 mmol/g at pH 4.7 could keep stable without creaming for 30 d. Furthermore, the GLT/BCNF 1.16, with the most remarkable emulsion stabilizing capacity, was successfully applied to prepare high internal phase emulsions with a more stable and higher viscoelastic behavior. This study was meaningful for the regulation of emulsion stability and rheological property.
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FOOD HYDROCOLLOIDS
·
2022
·
IF 11.504
Yuan Zhao,Zhongyang Ren,Linfan Shi,Wuyin Weng
The effects of incorporating a water-in-oil pre-emulsion based on different emulsifiers with similar hydrophilic-lipophilic balances on the physicochemical properties of soy protein isolate-based emulsion films were investigated. Confocal laser scanning microscopy images indicated that the oil droplet size in the polyglycerol polyricinoleate and lecithin pre-emulsions was larger than that in the glycerol monostearate, span, and sucrose ester pre-emulsions. By contrast, the oil droplet size in the film-forming emulsions had opposite orders. After drying, the polyglycerol polyricinoleate and lecithin emulsion films contained small and evenly distributed oil droplets and demonstrated a small difference of upper and lower surfaces in oil concentration and contact angle. The water vapor permeability of emulsion films prepared by polyglycerol polyricinoleate and lecithin pre-emulsion was 2.35 × 10 −10 g m −1 s −1 Pa −1 and 2.32 × 10 −10 g m −1 s −1 Pa −1 , respectively, lower than that of other emulsion films. The control emulsion films had the highest tensile strength of 7.43 MPa, whereas polyglycerol polyricinoleate emulsion films had the lowest tensile strength of 4.87 MPa. Furthermore, the polyglycerol polyricinoleate emulsion films had the lowest glass transition temperature among the prepared emulsion films. This study concluded that the properties of film-forming emulsions could be affected by pre-emulsions based on different emulsifiers, resulting in different physicochemical properties of the emulsion films.
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SENSORS
·
2019
·Vol. 19
·期 3
·674
·
IF 3.031
Hong Zhai,Yunfeng Bai,Jun Qin,Feng Feng
A novel colorimetric and ratiometric fluorescence sensor was constructed by using carbon quantum dots (CQDs) and o-diaminobenzene (ODB). Unlike ODB by itself, ODB oxide (oxODB) not only emits fluorescence, but also produces ultraviolet (UV) absorption. Therefore, on the basis of the potential optical properties of ODB, glucose oxidase (Gox) and horseradish peroxidase (HRP) were introduced into a CQDs–ODB system for the quantitative oxidation of ODB. When glucose is present, it is oxidized by oxygen under the catalytic action of its oxidase to form hydrogen peroxide. Hydrogen peroxide is a strong oxidant that can rapidly oxidize ODB through the catalysis of horseradish peroxidase. oxODB can cause changes in the fluorescence ratio (I550/I446) and absorbance ratio (A/A0). At the same time, the color of the detection solution can also change under sunlight and ultraviolet lamps. Therefore, glucose can be quantitatively detected by ratiometric fluorescence and colorimetry simultaneously, and semi-quantitatively detected by observing the colors with sunlight and ultraviolet lamps of 365 nm. This increases not only the convenience but also the accuracy of detection. In addition, this sensor has good selectivity and can be used for the determination of glucose in serum, providing a new idea for the development of blood glucose sensors.Keywords:dual-mode sensor;carbon quantum dots;o-diaminobenzene;glucose
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Journal of CO2 Utilization
·
2018
·
IF 5.503
Yu Cao,Ran Ma,Ning Wang,Mei-Yan Wang,Xue-Dong Li,Liang-Nian He
Selective hydrogenolysis is a crucial challenge for lignin valorization. A PdCl 2 -catalyzed hydrogenolysis of C OH bond of various lignin β-O-4 alcohol model compounds was developed for preparation of corresponding phenethoxybenzene in 78–98% isolated yield. Notably, the introduction of low-pressure CO 2 (1 MPa) remarkably improves the reaction efficiency and selectivity of phenethoxybenzene. Neither over-reduction of aromatic ring nor further debenzylation was detected. This is understandable that the in situ methylcarbonic acid generated from CO 2 and methanol acts as an acidic catalyst and enhances the leaving ability of hydroxyl group of β-O-4 alcohols. Besides, the present PdCl 2 /CO 2 /MeOH catalyst system proved to be effective for reductive cleavage of C O bonds of β-O-4 ketones, producing ethylbenzenes accompanied with phenols in high yields. Furthermore, this protocol could also be extended to selective hydrodeoxygenation of the carbonyl group to methylene in aromatic ketones. As a sound reaction medium, such in situ CO 2 /MeOH acidic system could be inherently neutralized by depressurizing CO 2 , providing feature advantages for simple post-processing and none waste disposal.
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NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 11
·9140-9150
·
IF 3.201
Jiliang Ma,Xinwen Peng,Linxin Zhong,Runcang Sun
The application of biomass-based carbonaceous solid acids in catalysis is attracting increasing attention in the field of chemistry. In this study, a heterogeneous carbon-based solid acid biocatalyst (CXH-SO3H) with regular spherical structure was synthesized from xylan-type hemicellulose (XH) by a simple two-step method. The catalyst was successfully applied in the synthesis of O- and N-heterocycles with yields of 80–99% and 60–97%, respectively. In view of environment and economy, CXH-SO3H shows the merits of environmental friendliness, easy operation, simple work-up, excellent yields, and the avoidance of use of organic solvents and expensive catalysts. Moreover, the as-synthesized solid acid catalyst could be used for several cycles without significant loss in its catalytic activity. The results of FT-IR, XRD, and SEM showed that no distinct differences in physico-chemical structures of CXH-SO3H were observed. Thus, the eco-friendly CXH-SO3H catalyst is a promising candidate for green synthesis of O- and N-heterocycles from low-cost feed-stocks and has good prospect in partially substituting commercially available solid and liquid acid catalysts and precious metal catalysts.
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RSC Advances
·
2019
·Vol. 9
·期 28
·15694-15702
·
IF 3.049
Lijing Nan,Jiao Li,Wanjun Jin,Ming Wei,Mengjun Tang,Chengjian Wang,Guiping Gong,Linjuan Huang,Ying Zhang,Zhongfu Wang
Mass spectrometry (MS) analysis combined with stable isotopic labeling is of great importance for quantitatively profiling abnormal sialylated O-glycans associated with disease development, but technically hindered by the poor releasing efficiency of O-glycans from glycoprotein or the labile nature of sialic acid residues at glycans. Herein, we developed an isotopic precursor based metabolic amplification and labeling (IPMAL) technique for relative quantitative profiling of the repertoire O-glycans between normal and tumor cells by ESI-MS. Two groups of cells were incubated with peracetylated benzyl-α-N-acetylgalactosamine (Ac3GalNAc-α-Bnd0) or a heavy labeled peracetylated benzyl-α-N-acetylgalactosamine (Ac3GalNAc-α-Bnd5) precursor respectively to amplify the repertoire of O-glycans as Bnd0/d5-O-glycans which could achieve the quantitative O-glycome analysis by ESI-MS after derivatization. The established method demonstrates desirable feasibility, accuracy (relative error (RE) ≤ 4.20%), reproducibility (coefficient of variation (CV) ≤ 7.61%, n = 3) and good quantitation linearity (R2 > 0.99, n = 3) for five Bn-O-glycans with 2 orders of magnitude. Finally, the method has been successfully applied to quantitative analysis of the repertoire O-glycome changes between normal human liver cell line L02 and human hepatoma cell line SMMC-7721. Moreover, the α-2,3/2,6 sialic acid isomers of Bn-O-glycans from these two cells have been further quantitatively distinguished when involved a sialic acid specific derivatization procedure.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2019
·
IF 4.175
Worku Lakew Kebede,Dong-Hau Kuo,Misganaw Alemu Zeleke,Kedir Ebrahim Ahmed
Environmentally toxic methylene blue organic pollutants are of more concerns due to their antagonistic effects on human health, animals, and plants, thus needs serious attention for their removal. For elimination purpose, the Sb-doped Mo(O,S) 3 oxy-sulfide nanoplate catalyst with different Sb contents was synthesized at low temperature of 95 °C via a facile method. The structural, morphological, chemical composition, optical properties , and electrical conductivity of the catalyst were characterized with different techniques. The photocatalytic performance of Sb-Mo(O,S) 3 at various Sb contents was investigated for the degradation of methylene blue dye under visible light irradiation using hydrogen peroxide as an effective electron scavenger to further accelerate the reaction. It was observed that the incorporation of Sb enhanced the catalytic activity. Sb-Mo(O,S) 3 -10 was the most efficient catalyst with excellent activity to degrade 99.7% of the dye within 60 min irradiation time. The degradation kinetics follows a pseudo-first-order reaction with a rate constant 8.78 × 10 −2 min −1 , which is 3-fold higher than that for Sb- Mo(O,S) 3 -0 catalyst. Sb-Mo(O,S) 3 -10 showed slower recombination of photogenerated charge carriers and lower charge transfer resistance which proved to be capable for the removal of toxic methylene blue organic pollutant.
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