CATALYSIS LETTERS
·
2021
·Vol. 152
·期 5
·1495-1505
·
IF 3.186
Zhang Yue,Wang Li,Ma Qingqing,Wang Nan,Pan Zhiyong
SBA-15 was modified via post-treatment with (NH 4 ) 2 SiF 6 and (NH 4 ) 3 AlF 6 solution (NSF-T and NAF-T) and applied as support of Pd catalysts for the hydrogenation of 2-ethyl-anthraquinone (EAQ). The characterization results revealed that F could be incorporated into the framework of SBA-15 by forming Si–F bond and the amount of F increased as the molar ratio of F in treating solution to Si species in SBA-15 (F/Si) increased from 0.1 to 0.4 for NSF-T and 0.3 to 0.6 for NAF-T. At the same F/Si, the incorporated amount of F was larger with NSF-T than with NAF-T, and the latter could simultaneously create acid sites in catalysts. The hydrophobicity of catalysts could be effectively improved by incorporating F into SBA-15 supports, which favored the catalytic performance. The catalyst on SBA-15 treated by NSF with F/Si of 0.3 exhibited the high initial activity (0.24 molH 2 ·gPd −1 ·min −1 ) and selectivity (95.5%). Graphic Abstract
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ChemSusChem
·
2021
·Vol. 14
·期 14
·2935-2942
·
IF 8.928
Jifang Zhang,Wanbing Gong,Huajie Yin,Dongdong Wang,Yunxia Zhang,Haimin Zhang,Guozhong Wang,Huijun Zhao
Graphical Keep it 100 : A facile immersion approach has been developed to grow ultrathin nickel hydroxide nanosheets, which show excellent performance as the anode for electrocatalytic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid with 100 % yield and essentially 100 % faradaic efficiency under a low potential within a short reaction time. Development of electrocatalysts that are capable of efficiently oxidizing biomass-derived 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) is critically important for production of degradable plastics via non-fossil routes. In this study, a facile and scalable immersion synthetic approach has been developed to grow ultrathin nickel hydroxide nanosheets in situ on commercial nickel foam (Ni(OH) 2 /NF) as an anode for the electrocatalytic oxidation of HMF to FDCA with complete HMF conversion, 100 % FDCA yield, and >99 % faradaic efficiency at 1.39 V (vs. RHE) within 90 min. Mechanistic studies reveal that the initial oxidation of HMF takes place at the carbonyl group and FDCA is generated through two further oxidation steps. Impressively, the synthesized Ni(OH) 2 /NF can also be used to electrocatalytically oxidize other alcohol/aldehyde-containing compounds to the targeted products in alkaline medium with 100 % yield and >94 % faradaic efficiency under a low oxidation potential of 1.39 V (vs. RHE) within short reaction times.
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Surfaces and Interfaces
·
2021
·
IF 4.837
Zhongxuan Xu,Diandi Li,Yuping Tan,Qinyu Yang,Han Xiong,Jiguang Li,Hong Deng,Zhang Lin
Microbial treatment of heavy metals is a low-cost and environmentally friendly method. During the treatment of chromium pollution, environmental media has a great impact on the efficiency of bacteria Cr immobilization. However, when Cr(VI) coexist with different metal cations , the reduction of Cr(VI) and the immobilization of Cr by bacteria are still unclear. In our research, although bacteria were significantly promoted the reduction of Cr(VI) with the coexistence of Mn(II), the bacteria produced the maximum of soluble organic Cr(III). In the performance of immobilization Cr, Mg(II) group has the highest chromium immobilizing rate. In addition, Cd(II) has the strongest inhibitory effect on Cr(VI) reduction and Cr immobilization. The SEM results show that Cr were stored in the cells. However, XRD analysis did not demonstrate the crystal structure. Our research investigated the ability of bacteria to reduce and immobilize Cr with the coexistence of 9 different metal ions, and provided a reference for a deeper understanding of the relationship between bacteria and metal ions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Bo Lv,Xuefan Feng,Xiaoping Xi,Xinyan Feng,Zhenyu Yuan,Yu Yang,Fuqin Zhang
Heterogeneously structured materials with supported precious metals , such as Pd, Pt, and Ru, as co-catalysts are important catalysts for efficient photocatalytic water splitting. However, the high costs and low reserves of precious metals have been an obstacle to their application in hydrogen production . In this work, the noble-metal-free Cd 0.3 Zn 0.7 S solid solution was designed and synthesized with an optimized molar ratio of Cd/Zn for the best visible light photocatalytic performance. In addition, a heterojunction hybrid material formed between the Cd 0.3 Zn 0.7 S and Ni(OH) 2 nanosheet was engineered to improve the utilization of light and to inhibit the recombination of holes and electrons. Ni(OH) 2 nanosheets assisted the transfer of the photoexcited electrons to participate in the reduction reactions which is critical for efficient and rapid catalytic hydrogen production. The photoelectrochemical property of the hybrid material was investigated with UV–vis absorption, photoluminance (PL) and electrochemical impedance spectroscopy measurements. The mechanism of the high-efficiency and low-cost photocatalytic hydrogen production was established by analyzing the hydrogen evolution kinetics. With the success of replacing precious metal with nickel-based surface heterostructure, this work is expected to provide a new type of photocatalyst for the application of photocatalytic hydrogen production.
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RARE METALS
·
2021
·Vol. 41
·期 3
·889-900
·
IF 4.003
Wang Ting,Zhang Bin,Yin Chao-Qun,Zhao Jun,Liu Xiang,Wang Chuan
The selective hydrogenolysis of C–O bond in furfural and its derivatives provides a sustainable route for transforming biomass-derived feedstocks into valued chemicals. Currently, the development of efficient catalysts which can effectively cleavage C–O bond under mild conditions remains a critical challenge. The present work reports Pt catalysts supported on multi-walled carbon nanotubes (MWNT) which are active in 2-methylfuran (2-MF) hydrogenolysis to form pentanols in liquid phase under mild conditions. The impact of various catalyst supports, active metals and reaction conditions in terms of metal loadings, solvent, time, pressure, etc., were explored. The 5 wt% Pt/MWNT catalyst demonstrated an excellent activity and selectivity with 100% 2-MF conversion and 53% pentanols (POLs) yield under 1 MPa H 2 at an exceptional low temperature of 25 °C. The reaction mechanism was studied combing both the reactivity tests and characterization results, and it is found that the better catalytic performances of Pt/MWNT were correlated closely to the size of Pt nanoparticles and their interactions with the underlying MWNT support. Accordingly, a reaction pathway involving the adsorption of 2-MF parallel to the Pt nanoparticles and its subsequently selective C–O hydrogenolysis was proposed. This work showcases a promising catalyst for room-temperature biofuel production. Graphical abstract
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JOURNAL OF PHARMACY AND PHARMACOLOGY
·
2021
·Vol. 74
·期 4
·596-604
·
IF 3.765
Sun Liyun,Shang Huoli,Wu Yuzhen,Xin Xiujuan
ObjectivesThe combination of gemcitabine (Gem) and hypericin (HY) enhances the apoptosis of Capan-2 cells, providing a promising option for the treatment of pancreatic cancer. Our study further explored the cytotoxic mechanism of HY combined with chemotherapy drugs on pancreatic cancer.MethodsThe proliferation rate of the cells assayed with the MTT method. The ROS (reactive oxygen species) levels of each treatment were evaluated by DCFH-DA oxidisation methods. The activity of glutathione reductase and the levels of reduced glutathione (GSH) and oxidised glutathione (GSSG) were assessed using assay kits. The expression levels of apoptosis-related proteins were analysed by western blotting.Key findingsThe activity of glucose-6-phosphate dehydrogenase (G6PDH), a key enzyme of the pentose phosphate pathway, significantly decreased in Gem + HY groups, however, the ROS level enhanced accompanying with GSH depleting, mitochondrial membrane depolarisation and cytochrome C release. Gem + HY inhibits the expression of Bcl-2 but stimulates Bax level, triggering caspase activation and PARP cleavage and thus promoted apoptosis of Capan-2 cells.ConclusionsWe demonstrated that Gem combined HY-PDT could inhibit the proliferation of Capan-2 cells and induce cell apoptosis. HY-PDT combined with Gem had a great potential on pancreatic cancer treatment clinically.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Zhiguo Zhang,Hua Huo,Zhenjiang Yu,Lizhi Xiang,Bingxing Xie,Chunyu Du,Jiajun Wang,Geping Yin
Mn doping is deemed as a promising strategy to improve the electrochemical performance of the α-Ni(OH) 2 battery-type supercapacitor electrode. However, the internal structure evolution, the pathways and the dynamics of the proton/intercalated anion migration, as well as the functioning mechanism of Mn dopant to stabilize the layered structure during cycles remain unclear. Here, we unveil that irreversible oxidization of Mn 3+ at the initial CV cycles, which will remain as Mn 4+ in the NiO 2 slabs after the first oxidization to effectively suppress the phase transformation from α-Ni(OH) 2 /γ-NiOOH to β-Ni(OH) 2 /β-NiOOH and further maintain the structural integrity of electrode. With a synergistic combination of theoretical calculations and various structural probes including XRD and 2 H MAS solid state NMR, we decode the structure evolution and dynamics in the initial CV (cyclic voltammetry) cycles, including the absorption/desorption of hydrogen containing species, migration of intercalated anions/water molecules and the change of interlayer space. This present work elucidates a close relationship between doping chemistry and structural reliability, paving a novel way of reengineering supercapacitor electrode materials.
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JOURNAL OF CLUSTER SCIENCE
·
2020
·Vol. 32
·期 5
·1371-1379
·
IF 1.731
Zhang Yingzhen,Song Yingying,Li Yancai
A simple and environment-friendly autocatalytic reduction process was developed for synthesis of Au/Ni(OH) 2 nanocomposites. The nanocomposites were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). It is found the nanocomposites are composed of ultrathin Ni(OH) 2 nanosheets and gold nanoparticles (AuNPs), and the AuNPs disperse evenly on the Ni(OH) 2 nanosheets. The electrochemical and electrocatalytic properties of the Au/Ni(OH) 2 modified glassy carbon electrode (Au/Ni(OH) 2 /GCE) were investigated by electrochemical experiments. Furthermore, through optimizing Au loading of the nanocomposites, the 5%-Au/Ni(OH) 2 /GCE displays the best electrocatalytic activity towards glucose oxidization in alkaline medium. Under optimal conditions, the 5%-Au/Ni(OH) 2 /GCE displays a wide linear range of 0.01 to 3.15 mM (R 2 = 0.998) to glucose. Besides, the sensor has a low detection limit of 0.10 μM (S/N = 3) and a high sensitivity of 342.1 μA·mM −1 ·cm −2 . It also displays satisfying stability, good reproducibility and selectivity.
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ENERGY
·
2020
·
IF 6.082
Kun Fu,Chenxu Liu,Lemeng Wang,Xiayu Huang,Dong Fu
In this work, novel non-aqueous absorbents composed of 2-ethylhexan-1-amine (EHA) and glyme were proposed for CO 2 capture. The absorption performance of CO 2 in EHA + diglyme, EHA + triglyme and EHA + tetraglyme non-aqueous solutions was investigated and the viscosities ( η ) of the CO 2 -saturated absorbents were measured. Besides the experiments, kinetic models were applied to correlate the CO 2 absorption. The activation energy ( E a ) was obtained from Arrhenius equation , and the absorption mechanism was deduced. The results showed that both Lagergren model and Avrami model can accurately correlate and predict the time-dependent absorption amount, thus an optimized composition under which excellent absorption performance and relatively low η and E a can be simultaneously achieved was determined. Compared to water-based absorbents like MEA, the optimized non-aqueous absorbents take the advantages of better absorption performance and lower activation energy. Moreover, the glyme solvents have about 50% lower specific heat capacities and much higher boiling points (≥435 K) than water, which is expected to greatly reduce the sensible heat and the latent heat of the solvent during regeneration. Therefore, the proposed novel absorbents have promising industrial application potential in the CO 2 capture process.
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Nature Communications
·
2020
·Vol. 11
·期 1
·1-10
·
IF 12.121
Yang Qihao,Xu Wenwen,Gong Shun,Zheng Guokui,Tian Ziqi,Wen Yujie,Peng Luming,Zhang Linjuan,Lu Zhiyi,Chen Liang
Elucidating the structure-property relationship is crucial for the design of advanced electrocatalysts towards the production of hydrogen peroxide (H 2 O 2 ). In this work, we theoretically and experimentally discovered that atomically dispersed Lewis acid sites (octahedral M–O species, M = aluminum (Al), gallium (Ga)) regulate the electronic structure of adjacent carbon catalyst sites. Density functional theory calculation predicts that the octahedral M–O with strong Lewis acidity regulates the electronic distribution of the adjacent carbon site and thus optimizes the adsorption and desorption strength of reaction intermediate (*OOH). Experimentally, the optimal catalyst (oxygen-rich carbon with atomically dispersed Al, denoted as O-C(Al)) with the strongest Lewis acidity exhibited excellent onset potential (0.822 and 0.526 V versus reversible hydrogen electrode at 0.1 mA cm −2 H 2 O 2 current in alkaline and neutral media, respectively) and high H 2 O 2 selectivity over a wide voltage range. This study provides a highly efficient and low-cost electrocatalyst for electrochemical H 2 O 2 production.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Long Wang,Huali Jin,Min Wei,Wenjie Ren,Yurong Zhang,Liying Jiang,Tao Wei,Baoshan He
Herein, an electrochemical aptasensor was constructed for ultra-sensitive determination of T-2 toxin based on Silver ion (Ag + ) -dependent DNAzyme-assisted signal amplification and Gold nanoparticles/Graphene oxide @ manganese dioxide (AuNPs/MnO 2 @GO) nanocomposites. In the presence of Ag + , the secondary structure of the T-2 aptamer is altered via the Ag + mediated coordination of C–Ag + –C base pairs. When T-2 toxin is added, the secondary structure of DNA is changed again, and the trapped Ag + are released. Then, the DNAzyme could repeatedly bind and cleave methylene blue (MB)-modified substrate DNA (S-DNA) in the assistance of Ag + , which leads to a decrease in the electrochemical signal. With the optimal conditions, there is a good linear relationship between the current value and the logarithm of T-2 toxin concentration in the range from 2 fg mL −1 to 20 ng mL −1 , and a detection limit of 0.107 fg mL −1 is obtained. Moreover, the proposed method was successfully applied to measure T-2 toxin in beer, thus showing great potential of this system for food safety and quality control.
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BIOCHIMICA ET BIOPHYSICA ACTA-MOLECULAR BASIS OF DISEASE
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2020
·
IF 4.352
Jinfu Qian,Wu Luo,Chengyi Dai,Jun Wang,Xinfu Guan,Chunpeng Zou,Nipon Chattipakorn,Gaojun Wu,Weijian Huang,Guang Liang
Angiotensin II (Ang II)-induced vascular inflammation and injury entails endothelial to mesenchymal transition (EndMT). Recent studies have shown that Ang II engages toll-like receptor 4 (TLR4) in the vasculature to mediate adverse effects. Here, we aimed to investigate whether myeloid differentiation protein 2 (MD2), an extracellular molecule indispensable for TLR4 activation, mediates Ang II-induced vascular injury and EndMT. We utilized MD2 knockout mice and wildtype mice treated with a specific MD2 inhibitor to decipher its role in aortas of Ang II-challenged mice. To confirm our results and to provide mechanistic insights, we exposed cultured endothelial cells to Ang II, with or without MD2 silencing. We show that Ang II causes deleterious remodeling and EndMT in aortas of mice within two weeks. These Ang II effects were largely absent in MD2 knockout mice and in wildtype mice treated with a MD2 inhibitor. MD2 silencing in cultured endothelial cells confirmed the essential role of MD2 in Ang II-induced inflammatory factor induction, and EndMT-associated phenotypic change. We also found that Ang II-MD2-EndMT axis involves the activation of nuclear factor-κB. Our studies highlight an essential role of MD2 in Ang II-induced vascular inflammation and EndMT contributing to vascular injury. These results also imply that MD2 may be targeted to dampen inflammatory cardiovascular and EndMT-associated diseases.
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