International Journal of Electrochemical Science
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2023
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IF 1.5
Yanyan Xu,Wenwen Xiao,Pengli Ge,Wenguang Zeng,Qingshan Liu,Zhengyuan Gao,Yongbo Yan
This work aimed to develop a high-efficiency and reliable alternative for conventional and toxic corrosion inhibitor. A novel tetrazole derivative (1-Phenyltetrazole-5-thiol, PTT) that possessed excellent anti-corrosion capacity was exploited for the first time. Based on the traditional electrochemical investigation, morphological observation, and computer modeling, inhibition ability and adsorption type of PTT for X70 steel in 0.5 M H 2 SO 4 were varied. The electrochemical results showed that PTT was a mixed organic inhibitor, which could retard charge transfer impedance, and slowed down the corrosion rate of steel. Specifically, the highest inhibition efficiency was 95.1% when the added PTT dose was 2 mM. The adsorption model showed that the PTT film was formed via powerful physicochemical adsorption. As shown in theoretical calculations, the lower Δ E , higher μ values and E binding value of PTT corresponded to supreme adsorption performance, which was also a manifestation of the PTT high-efficiency corrosion inhibition.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Huimin Li,Xinyuan Huang,Ye Lv,Jinli Zhang,Wei Li
The biomass electrochemical oxidation has attracted worldwide attention owning to its carbon-neutral and sustainable nature. Here, different morphologies of CoCu-carbonate hydroxides (CH) electrodes are prepared through one-step hydrothermal method for 5-hydroxymethylfurfural electrocatalytic oxidation (HMF-ECO) to high-valued 2,5-furandicarboxylic acid (FDCA) for the first time. The results illustrate that Cu can regulate CoCu–CH morphologies from 1D nanorods to 2D ultra-thin nanosheets besides modulating the catalytic compositions . The optimal Co 1 Cu 1 –CH exhibits hybrid nanostructures containing the 1D nanorods and 2D ultra-thin nanosheets , which has the largest ECSA and specific surface area, as well as the smallest Tafel slope and impedance. The oxidation potential of HMF-ECO is 1.42 V vs RHE with the conversion of HMF 99.57%, the selectivity for FDCA 99.91%, and the FE 98.88%. In addition, Cu can promote the conversion of Co 2+ to the favorable Co 3+ for HMF-ECO on the catalyst surface . Density functional theory calculation indicates that Cu can improve charges transfer to HMF and lower its adsorption energy . In situ Raman spectra tests indicate that cobalt species is the active site for HMF-ECO. Furthermore, at 1.42 V vs RHE, the coupling of HMF-ECO and hydrogen evolution reaction shows that the cathodic hydrogen evolution rate is 92.33 L h −1 m −2 , which is 3.69 times more than water splitting. This work provides a special structures material to process intensification of HMF electrooxidation coupling hydrogen production .
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FUEL
·
2022
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IF 8.035
Mengjiao Xing,Yunlei Chen,Jian Cao,Yuanlong Han,Zhichao Tao,Fei Wang,Kun Hao,Ling Zhang,Wentao Zheng,Hongwei Xiang,Yong Yang,Yongwang Li,Xiaodong Wen
Understanding the catalytic structure–activity relationship over active sites is of fundamental importance in heterogeneous catalysis field. Herein, a series of H-ZSM-5 zeolites with Al pairs contents in the range of 31% to 82% are used to explore the structure sensitivity of olefin aromatization reaction. Compared with high reaction temperatures (385 ℃ and above), prominently different initial aromatic yields are observed over the samples at 150 ℃. In addition, the 1-octene temperature-programmed surface reaction (TPSR) and theoretical calculation results give a thorough understanding on active site dependent activation temperature (100 vs 150 ℃ over Al pairs and single Al). However, the catalytic cycle of olefin aromatization is not sustainable at low reaction temperature, which is due to the formation and blocking of big molecules in the micropores (e.g., trimethylbenzene etc.). In conclusion, the desorption of big molecules is the rate-determining step for olefin aromatization reaction over H-ZSM-5, which masks the structure sensitivity over Al pairs and single Al.
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RESEARCH ON CHEMICAL INTERMEDIATES
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2022
·Vol. 48
·期 11
·4517-4536
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IF 3.134
Yang Zizhen,Wang Siya,Chen Ou,Wang Zhengwei,Xu Jundong,Zheng Shuqin
In this paper, FeMn-ZSM-5/MOR(FeMn-Z/M) catalyst was synthesized through in-situ crystallization and wet impregnation method and used as heterogeneous Fenton-like catalyst for degradation of indigo carmine (IC) in aqueous solution. The catalysts were characterized using XRD, BET, SEM, EDS, FT-IR and XPS techniques. The experimental results showed that Fe and Mn were successfully doped onto the ZSM-5/MOR(Z/M) surface. The combination of ZSM-5 and mordenite (MOR) not only enhanced the adsorption capacity of contaminant, but also had more active sites. Degradation experiments and the valence variations indicated that Fe and Mn had a significant synergistic effect. The results of IC degradation experiments under different conditions showed that the optimum conditions (FeMn mass ratio = 1:2, FeMn-Z/M = 25 mg, H 2 O 2 = 0.5 ml, pH = 3), the degradation rate of IC reaches 99% in 20 min. Reaction analyses showed that catalyst follow a first-order reaction kinetic. The degradation of IC could be divided into two stages: adsorption/oxidation (After adsorption, oxidative degradation begins) and Fenton-like reaction. Free radicals quenching studies analyzed verified that the dominant free radicals within FeMn-Z/M Fenton-like system were hydroxyl radical (·HO) and hydro-peroxy radical (·HO 2 ), ·HO 2 was the main free radical in the adsorption/oxidation stage. The possible catalytic mechanism was proposed. Finally, the synthesized FeMn-Z/M catalyst had better performance than other IC removal methods, and had good degradation efficiency and high reusability after multiple runs.
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JOURNAL OF ORGANIC CHEMISTRY
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2022
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IF 4.198
Jun Ma,Qijie Zou,Chunhua Wang,Guangwei Yin,Fangyi Li
Herein, we report a base promoted dibromination of enamides using CBr4 as a bromine source to provide expedient access to β,β-dibrominated secondary enamides. Preliminary synthetic application study shows that these novel products can be readily transformed to 5-Br oxazoles via Cu(I) catalyzed intramolecular cyclization in good yields.
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PubMed
高影响因子
DALTON TRANSACTIONS
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2022
·Vol. 51
·期 48
·18473-18479
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IF 4.569
Yan Zhou,Shanshan Lv,Han Li,Qikang Wu,Taiyu Chen,Shaohuan Liu,Wanying Li,Wenjuan Yang,Zheng Chen
The development and transformation of biomass-derived platform compounds is a sustainable way to deal with the fossil fuel crisis. 5-Hydroxymethylfurfural (HMF) can be reduced or oxidized to produce many high-value compounds; however, it is challenging to effectively produce 2,5-diformylfuran (DFF) due to overoxidation. In this work, a carbon-doped V2O5 (C–V2O5) material was obtained through pyrolysis of MIL-47(V) nanorods, a typical metal–organic framework material. The X-ray diffraction patterns and X-ray photoelectron spectra showed that the graphitized carbon species were incorporated in C–V2O5. High-efficiency HMF oxidation, high specific selectivity for DFF and excellent recycling could be achieved with the C–V2O5 catalyst. Fourier-transform infrared spectroscopy combined with density functional theory (DFT) calculation revealed that graphitized carbon weakens the VO bond and promotes the formation of oxygen vacancies in C–V2O5, thus improving the catalytic activity in the oxidation of furfuryl alcohols. The V4+ induced by oxygen vacancies will be oxidized by O2 to form V5+, so that the cycle can be realized. It exhibits remarkable selectivity in the oxidation of different alcohols produced from biomass based on the relatively constant active sites in C–V2O5.
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PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Chenxi Lu,Yuanzhuo Zhou,Liangzhi Li,Hongwei Chen,Lishi Yan
Catalytic production of 5-hydroxymethylfurfural (5-HMF) from glucose is a promising routine for generation of varied value-added chemicals. Herein, Mixed-Metal metal–organic frameworks (MOFs)–Fe/MIL-101(Cr) and MIL-101(Cr, Fe) obtained from post-synthesis modification and one-pot synthesis approach respectively were applied for catalytic converting glucose to 5-HMF. The synthesized Mixed-Metal MOFs were characterized by PXRD, SEM, N 2 adsorption–desorption analysis, TGA, XPS and NH 3 -TPD. Cr-and Fe-containing Mixed-Metal MOFs Fe/MIL-101(Cr) and MIL-101(Cr, Fe) presented synergistic effect with enhanced catalytic ability for glucose transformation to 5-HMF compared with typical single-metal MOFs and sulfonic acid-functionalized MOFs. Moreover, these two Mixed-Metal MOFs also presented better thermal stability than single-metal MOFs like MIL-101(Cr). Fe/MIL-101(Cr) was found to possess higher catalytic performance than MIL-101(Cr, Fe). 55.8 % 5-HMF yield was obtained with Fe/MIL-101(Cr) at 170 °C for 2 h in DMSO/water system. In addition, Fe/MIL-101(Cr) demonstrated desired recyclability for five times without incredible loss in its activity. This study provides a Mixed-Metal strategy on MOFs for improving catalytic efficiency of glucose conversion to 5-HMF.
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MATERIALS CHEMISTRY AND PHYSICS
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2022
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IF 4.778
Haotian Guo,Xinhuan Lu,Jie He,Huaxin Zhang,Haifu Zhang,Yanhong Dong,Dan Zhou,Qinghua Xia
A composite material ZSM-5@Co-MOF containing Co-MOF and ZSM-5 was successfully prepared by steam-assisted crystallization of Co-MOF on the zeolite surface. Compared to physically mixing Co-MOF on the zeolite surfaces, Co-MOF nanosheets were uniformly attached to external surfaces of the ZSM-5 crystals because of the enhanced interaction between zeolite and Co-MOF in the composite. In addition, the Co-MOF was distributed as a nanosheet structure, and its dispersibility was greatly enhanced, in which this behavior led to more uniform distribution of the deposited active sites. Interestingly, the designed composite exhibited an excellent catalytic performance for the epoxidation of α-pinene with air. Compared to isolated Co-MOF and ZSM-5, high yield of the product (94.4%) was obtained over the 0.5ZSM-5@Co-MOF-150 composite due to the highly dispersed Co-MOF nanosheet. This opens up interesting prospects for developing new zeolite@MOF composite catalysts as efficient heterogeneous catalysts.
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Advanced Materials Interfaces
·
2022
·Vol. 9
·期 35
·2201688
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IF 6.389
Liu-Qin Zhang,Hua-Li Li,Xiao-Hu Zhang,Qiu-Ping Li,Shu-Wen Luo,Fa-Qian Liu
Metal–organic gels or metallogels (MOGs), which usually made up with metal ions and organic ligands, are promising in the area of medicine, environment, and biology. Herein, a new metal–organic gel containing Cu + (Cu-MOG-5) is prepared at room temperature using 2-amino-5-mercapto-1,3,4-thiadiazole (AMT) and CuI. Considering the excellent low surface energy characteristics of polydimethylsiloxane (PDMS), the as-prepared Cu-MOG-5 is infused into porous PDMS to obtain Cu-MOG-5/PDMS coating, which combines the bactericidal properties of Cu + containing hydrogels and the low surface energy of PDMS. The morphology of the Cu-MOG-5 and Cu-MOG-5/PDMS coating is investigated by FE-SEM, and the structure of the new Cu-MOG-5 is verified by FT-IR, 1 H NMR, XPS, EDS, and elemental analysis. The antibiofouling properties are assessed using Escherichia coli ( E. coli ) and mussel. The results show that the newly prepared Cu-MOG-5/PDMS coating exhibits superior antibiofouling performance because of the synchronous action of hydrogel including Cu + and PDMS.
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Sustainable Energy & Fuels
·
2022
·Vol. 6
·期 23
·5281-5289
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IF 6.813
Zhefei Zhao,Xingyu Luo,Jiaxi Peng,Siqi Wang,Tianyang Guo,Huajun Zheng
Electrocatalytic conversion of biomass-derived platform molecules is regarded as an emerging approach to obtain high-value fuels and chemicals. Herein, a heterostructured design strategy involving dispersed Ag nanoparticles immobilized on one-dimensional TiO2 nanotubes (Ag-TiO2 NTs) for the electroreduction of 5-hydroxymethylfurfural (HMF) into 2,5-dihydroxymethylfuran (DHMF) was reported. The optimal electrode exhibited an 82.2% FE, 89.8% selectivity, and DHMF productivity value of 0.1 mmol cm−2 h−1. Electrochemical measurements combined with density functional theory (DFT) calculations manifested that the superior performance was derived from the heterojunction-induced metal–semiconductor interactions at the interface, by which the TiO2 NTs and Ag bring complementary advantages inhibiting the hydrogen evolution reaction (HER) and facilitating charge transfer. Moreover, the catalytic activity of the Ag sites on Ag-TiO2 NTs was considered separately. The mass activity of Ag on Ag-TiO2 NTs reached 5.8 mol L−1 g−1, which was far more than that of Ag mesh (0.038 mol L−1 g−1), indicating the significantly enhanced activity of Ag with high utilization. This could be attributed to the controllable nucleation of Ag through the confinement effect of TiO2 NTs, acquiring dispersed Ag nanoparticles. The design scheme for the heterostructured Ag-TiO2 NTs electrocatalyst displays prospective applications for developing highly efficient electrocatalysts for the electrochemical reduction of HMF.
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JOURNAL OF MOLECULAR LIQUIDS
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2022
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IF 6.633
Pengrui Zhang,Ciming Wang,Zixuan Xue,Lianjing Mao,Jinhe Sun,Fei Shao,Mixiang Qi,Yan Jing,Yongzhong Jia
Controlled fusion energy is considered to be one kind of sustainable energy source with clean and green properties. The fusion process requires a large number of lithium isotopes, but the naturally stable lithium isotopes 6 Li and 7 Li cannot be directly applied to the fusion process and must be further enriched. In this paper, a system for the separation of lithium isotopes by extraction was investigated, which mainly consists of bromobenzene-15-crown-5 and ionic liquids. The effects of ionic liquids, lithium salts, crown ether concentration, and temperature on the separation performance of lithium isotopes were explored. It was found that 6 Li was enriched in the organic phase and the single-stage separation factor reached 1.032. It was proved by the temperature experiment that the exchange of lithium isotopes was a spontaneous and exothermic process. The complexation ratio of crown ether and lithium ions was 1:1. The optimized complexation model and the interaction of crown ether and lithium ions were calculated by DFT and Multiwfn. Lithium ions were weakly bonded to the crown ether and strongly bonded to the water molecule as demonstrated by the non-bonded interactions and Mayer bond order of Li-O. Meanwhile, the mechanism of lithium isotope separation with crown ether was clarified by mutual verification of experiment and theoretical calculations.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jian Tian,Chuanhu Wang,Junwei Wu,Daohua Sun,Qingbiao Li
Pt works particularly well as a nanoparticle catalyst in the elimination of atmospheric pollutants, but its application is severely hampered by agglomeration and even poisoning in the presence of moisture. Hereby, a novel catalyst Pt@O-ZSM-5@OTS was synthesized to protect Pt, namely 0.5 wt% Pt was integrated into hollow ZSM-5 and subsequently coated hydrophobic octadecyltrichlorosilane (OTS) akin to the waterproof carapace. With the aid of various characterization techniques, the hybrid catalyst induced multiple marked features, such as dual-shell structure, hydrophobic microenvironment, and encapsulated active sites. Under excessively humid conditions (10 vol% H 2 O), the optimized Pt@O-ZSM-5@OTS2 exhibited a stable benzene conversion efficiency of 100 % for 120 h and outperformed the catalysts reported so far. Even reducing the reaction temperature to 170 °C, the conversion of benzene also reached 85 %, far exceeding the performance of untreated Pt@O-ZSM-5 (∼50 %). The outstanding stability stems from the hollow structure and OTS shell, which not only provide Pt with a protective shield against active site coverage, but also enhance competitive adsorption to benzene. Furthermore, DFT simulations unveil that the hydrophobic OTS shell enhances water resistance, consequently facilitates the oxidative degradation of contaminants at the active site. This work sheds light on novel strategies for the preservation of Pt by hydrophobic zeolite structures, as well as a deeper understanding of the elimination of aqueous VOCs.
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