APPLIED CATALYSIS A-GENERAL
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2023
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IF 5.5
Jiasheng Wang,Qingrong Wang,Mengdi Zhao,Ming Bao
Toluene gas-phase oxidation is a green, chlorine-free production process for benzaldehyde but its conversion efficiency is still unsatisfying due to the lack of highly efficient catalyst. Here the selective oxidation of toluene to benzaldehyde over V-Ag-Ce/TiO 2 under an air atmosphere was investigated. The catalyst was prepared by impregnation and characterized by scanning electron microscope (SEM), N 2 adsorption-desorption, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Electron paramagnetic resonance (EPR), H 2 temperature programmed reduction (H 2 -TPR), O 2 temperature programmed desorption (O 2 -TPD), and NH 3 temperature programmed desorption (NH 3 -TPD). The amount of oxygen vacancy and acid of the catalyst can be tuned through adjusting the V:Ag:Ce ratio. Over the optimum catalyst (V:Ag:Ce = 4:2:1, molar ratio), 92% benzaldehyde selectivity with a 27% toluene conversion can be obtained at 550 °C. Medium amounts of oxygen vacancy (0.43) and acidity (0.10 mmol/g) are found to be conducive to the conversion of toluene to benzaldehyde. This study has important theoretical guiding significance for improving conversion efficiency from toluene to benzaldehyde by gas-phase aerobic oxidation.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lulu Chen,Xiaona Dong,Ruonan Feng,Wanying Li,Dahu Ding,Tianming Cai,Canlan Jiang
Triclosan (TCS) is a compound in pharmaceutical and personal care products (PPCPs) that preferentially accumulates in soil and may threaten human health. Iron-based persulfate activation processes (Fe-PAPs) are a promising technique in soil remediation but are limited by their narrow pH application range and resultant iron precipitation. In this study, oxalic acid (OA) was specifically introduced to improve the efficiency of Fe 2+ -activated persulfate (PS) processes for TCS degradation in soil. The complexation of OA and Fe 2+ improved the total iron concentration in the Fe 2+ /OA/PS system and prevented iron precipitation. Fe-minerals in soil were also dissolved by OA, which participated in PS activation. The most appropriate proportion of Fe 2+ /OA/PS is 1:1:1, and approximately 85% of the TCS was degraded within 240 min compared with 45% in the Fe 2+ /PS system. SO 4 • - and 1 O 2 played important roles on TCS oxidation, while O 2 • - and CO 2 • - mainly participated in the iron cycle. The weak stretch of Fe-O in OA containing treatments in ATR-FTIR measurements provided evidence that OA dissolved the Fe-minerals. The introduction of OA in the Fe 2+ /PS system in four different soils reduced the negative effect of soil organic matter on TCS degradation. Three types of intermediates including hydroxylation, cleavage of ether bonds and cyclization products, were identified by LC-Q-TOF-MS. Column experiments were used to study the feasibility of in situ chemical oxidation (ISCO) remediation of TCS in the Fe 2+ /OA/PS system. Our findings indicated the ability of OA to be used as a cheating agent in Fe-PAPs for TCS soil remediation.
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EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
·
2023
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IF 6.7
Jianv Wang,Jing Jia,Qingqing He,Yang Xu,Hongye Liao,Xia Xiong,Li Liu,Changzhen Sun
Recent advancements in tumour-targeted therapies and immunotherapy offer hope to patients with various malignancies. However, the uncontrolled growth and metastatic infiltration of malignant tumours remain a huge therapeutic challenge. Therefore, this study aimed to develop an integrated multifunctional diagnostic and treatment reagent IR-251 that can not only be used for tumour imaging but also to inhibit tumour growth and metastasis. Besides, our results showed that IR-251 targeted and damaged the mitochondria in cancer cells via organic anion-transporting polypeptides . Mechanistically, IR-251 induced ROS overproduction by inhibiting PPARγ and then inhibiting the β-catenin signalling pathway and downstream protein molecules related to the cell cycle and metastasis. Moreover, the excellent anti-tumour proliferation and metastasis ability of IR-251 were verified in vitro/in vivo . And histochemistry staining revealed that IR-251 inhibited tumour proliferation and metastasis, which showed no significant side effect. In conclusion, this novel, multifunctional, mitochondria-targeting near-infrared fluorophore probe IR-251 has great potential in achieving accurate tumour imaging and inhibiting tumour proliferation and metastasis, and the underlying mechanism of action of IR-251 is mainly via the PPARγ/ROS/β-catenin pathway.
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高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Chen Sai,Luo Ran,Zhao Zhi-Jian,Pei Chunlei,Xu Yiyi,Lu Zhenpu,Zhao Chengjie,Song Hongbo,Gong Jinlong
Propane dehydrogenation (PDH) is an industrial technology for direct propylene production which has received extensive attention in recent years. Nevertheless, existing non-oxidative dehydrogenation technologies still suffer from the thermodynamic equilibrium limitations and severe coking. Here, we develop the intensified propane dehydrogenation to propylene by the chemical looping engineering on nanoscale core-shell redox catalysts. The core-shell redox catalyst combines dehydrogenation catalyst and solid oxygen carrier at one particle, preferably compose of two to three atomic layer-type vanadia coating ceria nanodomains. The highest 93.5% propylene selectivity is obtained, sustaining 43.6% propylene yield under 300 long-term dehydrogenation-oxidation cycles, which outperforms an analog of industrially relevant K-CrO x /Al 2 O 3 catalysts and exhibits 45% energy savings in the scale-up of chemical looping scheme. Combining in situ spectroscopies, kinetics, and theoretical calculation, an intrinsically dynamic lattice oxygen “donator-acceptor” process is proposed that O 2- generated from the ceria oxygen carrier is boosted to diffuse and transfer to vanadia dehydrogenation sites via a concerted hopping pathway at the interface, stabilizing surface vanadia with moderate oxygen coverage at pseudo steady state for selective dehydrogenation without significant overoxidation or cracking.
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LANGMUIR
·
2023
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IF 3.9
Ruixin Song,Shifei Kang,Liangtao Yao,Lulu Zheng,Dechao Yu,Dawei Zhang
BiVO4 has been widely used in the field of photocatalysis due to its nontoxic and moderate band gap. However, single BiVO4 has the disadvantages of a high recombination rate of photogenerated carriers and weak response to visible light, inhibiting its photocatalytic applications. To explore viable solutions, a hybrid material composed of lanthanum-doped bismuth vanadate (La-BiVO4) and oxygen-doped porous graphite carbon nitride (O-doped g-C3N4), i.e., La-BiVO4/O-doped g-C3N4 powder, was prepared by a facile hydrothermal reaction and low-temperature calcination. Then, the powder was loaded on polyacrylonitrile nanofibers (NFs) through the electrospinning fiber technique. Various surface science characterizations, including transmission electron microscopy and nitrogen absorption and desorption analysis, confirmed the successful synthesis of a mesoporous heterojunction material. The La3+-doping as well as the porous morphologies and larger specific surface area of the O-doped g-C3N4 ultimately improve the photocatalytic abilities via a proposed Z-scheme heterojunction mechanism. The roles of La3+-doping and morphology modification in promoting the separation of the photogenerated carriers and broadening the optical absorption range were experimentally discussed. The RhB degradation experiment indicated that the La-BiVO4/O-doped g-C3N4 powder has excellent photocatalytic activity, which is about 2.85 and 2 times higher than that of the pure BiVO4 and O-doped g-C3N4, respectively. Meanwhile, the La-BiVO4/O-doped g-C3N4 NF shows good stability and recoverability after a 10-cycle testing. Such a hybrid photocatalyst with a proposed Z-scheme heterojunction mechanism and good plasticity might pave a feasible way to fabricate a new library of photocatalysts.
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Advanced Science
·
2023
·Vol. 10
·期 18
·2207728
·
IF 15.1
Shibo Sun,Liwei Fang,Hui Guo,Liping Sun,Yong Liu,Yuanhui Cheng
All vanadium flow batteries (VFBs) are considered one of the most promising large-scale energy storage technology, but restricts by the high manufacturing cost of V 3.5+ electrolytes using the current electrolysis method. Here, a bifunctional liquid fuel cell is designed and proposed to produce V 3.5+ electrolytes and generate power energy by using formic acid as fuels and V 4+ as oxidants. Compared with the traditional electrolysis method, this method not only does not consume additional electric energy, but also can output electric energy. Therefore, the process cost of producing V 3.5+ electrolytes is reduced by 16.3%. This fuel cell has a maximum power of 0.276 mW cm −2 at an operating current of 1.75 mA cm −2 . Ultraviolet–visible spectrum and potentiometric titration identify the oxidation state of prepared vanadium electrolytes is 3.48 ± 0.06, close to the ideal 3.5. VFBs with prepared V 3.5+ electrolytes deliver similar energy conversion efficiency and superior capacity retention to that with commercial V 3.5+ electrolytes. This work proposes a simple and practical strategy to prepare V 3.5+ electrolytes.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Hefei Wang,Zeming Wang,Jibao Deng,Jian Wang,Yanzheng Gao
With low bioaccessbility, persistence of the undissolved organic pollutants in soil and sediments poses threat to health of the resident. Although ubiquitous black carbon catalyzes a wide range of biogeochemical reactions in nature, its role in biotransformation of the compounds in non-aqueous phase like 2, 2′-nitrobiphenyl remains unclear. Reduction rate constants of 2, 2′-dinitrobiphenyl by Shewanella oneidensis MR-1 increased from 0.0044 h −1 by 7-fold to 0.035 h −1 in the presence of black carbons produced at pyrolysis temperature of 250–900 °C. Accordingly, electrical conductivity of black carbon was enhanced from 0 to 5.56 S∙cm −1 . The reactivity of black carbon for catalyzing the biotransformation positively correlated with its electrical conductivity ( R 2 > 0.89), which was strongly associated with conductive graphitic clusters in it. The surface oxygenated groups in black carbon were likely not involved in the bioreduction. This work attaches importance to role of the ubiquitous black carbon in natural biotransformation of the undissolved pollutants, and elucidates new mechanism for the biotransformation.
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CORROSION SCIENCE
·
2023
·
IF 8.3
Aiying Chen,Jungan Jiang,Xiang Li,Juan Hou,Zhiyi Ding,Bin Gan,Kai Zhang
Thin-walled stainless steel (SS) bipolar plate (BP) with a star-shape flow field was fabricated by powder bed fusion (PBF). The full-scaled microstructure analysis was carried out to explore the relationship of cooling rate with the morphology evolution. The high cooling rate results in special nanotwins and stacking faults, together with different types of nano-inclusions. The printed PBFed samples deliver excellent corrosion resistance , surface conductivity and hydrophobicity in the simulated environment of proton-exchange membrane fuel cell. The enhanced corrosion resistance can be attributed to the thicker passivation film promoted by the ultra-fined grains, nano-scaled cluster cells, and nanotwins.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xinxin Zhang,Xiaota Cheng,Yang Si,Jianyong Yu,Bin Ding
As promising candidates for a wide range of applications, advanced ceramic aerogels with robust mechanical properties are urgently needed. However, the generic structural characteristics of ceramic aerogels, such as brittleness, fatigue failure, and large energy dissipation, present a great obstacle to their practical applications. Herein, we report a universal strategy to demonstrate a ceramic nanofibrous aerogel with superior elasticity and high fatigue resistance, realized by assembling flexible ZrO 2 -SiO 2 nanofibers into fluffy lamellar arch-shaped cellular structured. The as-obtained ZrO 2 -SiO 2 nanofibrous aerogels can rapidly recover from 90% strain, and exhibit high compression strength of 950 kPa (90% strain) and temperature-invariant superelasticity (from −196 to 1100 °C). In particular, the aerogels exhibit a low energy loss coefficient (0.28) and high fatigue resistance with zero plastic deformation after 1000 compression and release cycles, surpassing the performance of previously reported ceramic aerogels. Furthermore, the low thermal conductivity (0.0268 W m −1 K −1 ) and excellent high-temperature thermal insulation make it a desirable candidate for heat insulators under harsh conditions. The successful synthesis of these structural ceramic materials with high superelasticity, excellent compressibility, and superior fatigue resistance simultaneously opens up avenues for further the development of mechanically robust aerogel materials.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
·
IF 4.464
Xiaomei Ning,Xiaosong Zhou,Jin Luo,Liang Zhan
Pt modified by Bi had a great improvement for its catalytic performances. Herein, Bi-modified Pt was directly supported on carbon cloth (CC) as an efficient flexible electrode without using polymer binder. The catalyst structure of CC-based electrodes and their catalytic performances in glycerol and formic acid electro-oxidation reactions (GOR and FOR) were systematically studied. The research results indicated that Bi blocked certain sites of Pt, which limited the formation and adsorption of toxic products and intermediates. Bi-modified Pt on CC electrode had higher current density, better stability, and improved selectivity of dehydrogenation process in FOR and higher selectivity of glyceric acid in GOR. The electron enriched Pt resulting from Bi electron transfer and the increased bismuth hydroxide were in favor of the electro-oxidation catalytic performances. On the basis of introducing Bi, the added glucose was further beneficial to the performance due to the improved interaction between metal and CC.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Shahi Mulk,Muhammad Sajid,Lei Wang,Feng Liu,Gang Pan
5-Hydroxymethylfurfural (HMF) is one of the promising chemicals, which can serve as a platform chemical to produce various energy chemicals. HMF can be produced from different lignocellulosic biomass derived sugars employing different catalytic processes. In this study, the synthesis of HMF was investigated from excessively available sucrose using environment friendly and cost-effective technology . Among the various solvents applied, dimethyl sulfoxide (DMSO) was found as an efficient organic solvent medium. The results elucidated the combination of p -toluenesulfonic acid ( p TSA) and chromium chloride (CrCl 3 .6H 2 O) as the best dehydrating catalyst. A relatively higher HMF yield of 55% was achieved at a lower temperature (120 ℃) while at 150 ℃ (higher temperature) oxalic acid with higher concentration of CrCl 3 .6H 2 O gave a maximum yield of 59.21%. The time, temperature, and concentrations affected the yields. The positive impact was found with a rise in temperature from 100 to 120 ℃ in p TSA while oxalic acid affected the yield until 150 ℃. HMF yields were reported in descending order as p TSA > oxalic acid > maleic acid > malonic acid > succinic acid > blank at 120 ℃. It was observed that the isomerization of glucose to fructose is the major barrier to achieve the high process yield. Therefore, more efforts should be made to achieve the high rate of isomerization of glucose (part of sucrose disaccharide) in order to improve the HMF selectivity by depressing the humin formation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yangzhi Xu,Zirui Gao,Yao Xu,Xuetao Qin,Xin Tang,Zhiwei Xie,Jinrong Zhang,Chuqiao Song,Siyu Yao,Wu Zhou,Ding Ma,Lili Lin
Hydrogenation of CO 2 into methanol at low-temperature on Cu-based catalysts is of great significance, but remains challenging to enhance activity. In this paper, we report an inverse catalyst constructed with nano-ZrZnO x supported on Cu particles with outstanding methanol synthesis performance at 220 ℃, two times higher than that of commercial Cu/ZnO/Al 2 O 3 catalysts under the same conditions. Detailed structure characterization and performance evaluation demonstrate that the ZrZnO x mixed oxide serves as the most active oxide-metal interface site for CO 2 hydrogenation. The ZrZnO x /Cu inverse catalyst increases the weak and medium CO 2 adsorption sites which are further demonstrated responsible to the methanol productivity. In situ DRIFTs studies reveal that the inverse interface accelerates the reduction of asymmetric formate intermediates and prevents the generation of CO. The combination of enhanced CO 2 activation capability and accelerated hydrogenation rate of intermediates over the ZrZnO x /Cu inverse catalyst probably contribute to the remarkable methanol synthesis performance from CO 2 .
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