CHINESE JOURNAL OF CATALYSIS
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2021
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IF 8.271
Fang Li,Xiaoyang Yue,Haiping Zhou,Jiajie Fan,Quanjun Xiang
The active site amount of photocatalysts, being the key factors in photocatalytic reactions, directly affects the photocatalytic performance of the photocatalyst. Pristine graphitic carbon nitride (g-C 3 N 4 ) exhibits moderate photocatalytic activity due to insufficient active sites. In this study, cyano-modified porous g-C 3 N 4 nanosheets (MCN-0.5) were synthesized through molecular self-assembly and alkali-assisted strategies. The cyano group acted as the active site of the photocatalytic reaction, because the good electron-withdrawing property of the cyano group promoted carrier separation. Benefiting from the effect of the active sites, MCN-0.5 exhibited significantly enhanced photocatalytic activity for CO 2 reduction under visible light irradiation. Notably, the photocatalytic activity of MCN-0.5 was significantly reduced when the cyano groups were removed by hydrochloric acid (HCl) treatment, further verifying the role of cyano groups as active sites. The photoreduction of Pt nanoparticles provided an intuitive indication that the introduction of cyano groups provided more active sites for the photocatalytic reaction. Furthermore, the controlled experiments showed that g-C 3 N 4 grafted with cyano groups using melamine as the precursor exhibited enhanced photocatalytic activity, which proved the versatility of the strategy for enhancing the activity of g-C 3 N 4 via cyano group modification. In situ diffuse reflectance infrared Fourier transform spectroscopy and theoretical calculations were used to investigate the mechanism of enhanced photocatalytic activity for CO 2 reduction by cyano-modified g-C 3 N 4 . This work provides a promising route for promoting efficient solar energy conversion by designing active sites in photocatalysts.
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CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
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2021
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IF 1.134
Xu JING,Hao-Yue XUE,Xin HUANG,Hui-Yuan LI,Xiao-Wen WANG,Li-Yan JIA
A simple, efficient and environmentally-friendly pretreatment technique was proposed for determination of alkylphenols (4- tert -octylphenol, nonylphenol and octylphenol) in drink samples using high performance liquid chromatography-fluorescence detection. In this approach, the extractants in the form of (green) medium-chain fatty acids were generated in situ in the Pasteur pipette and extractant droplets dispersed by CO 2 generated by an effervescent reaction. A demulsifier was then used to break up the emulsion and induce phase separation, thus avoiding the need for a time-consuming centrifugation step. Finally, the floating extractant droplets were collected through solidification. Under optimal conditions, a good linearity was obtained in the concentration range from 0.1 μg/mL to 10 μg/mL, with determination coefficients ranging from 0.997 to 0.999. The extraction recoveries varied from 75.8% to 94.4% and the limits of quantification were in the range of 1.55–2.30 μg/L. The developed approach had good prospects in detection of alkylphenols in mineral water, tea drink, carbonated drink and Baijiu.
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CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
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2020
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IF 0.936
Hai XU,Pan ZHANG,Shao-Yan ZHOU,Qiong JIA
A magnetic molecularly imprinted polymer (MIP) was synthesized for the adsorption of methylene blue (MB). Magnetic particles were fabricated with fullerenes, which increased the surface area and provided a delocalized π-conjugate structure to enhance the hydrophobicity. A novel functional monomer with double carboxyl groups was designed based on the substituent reaction of methacryloyl chloride and iminodiacetic acid. The magnetic surface MIP was obtained with the functional compound as monomer, MB as template, and 2-vinylbenzene as crosslinker. The maximum adsorption amount was calculated to be 41.5 mg/g. The adsorption isotherm results revealed that this enrichment process followed Freundlich isotherm model and the adsorption kinetics could be well described with pseudo-second-order equation. The adsorption behavior was multilayer and mainly driven by chemical adsorption.
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CHINESE JOURNAL OF CATALYSIS
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2020
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IF 6.146
Nian Hu,Xiao-Yun Li,Si-Ming Liu,Zhao Wang,Xiao-Ke He,Yue-Xin Hou,Yu-Xiang Wang,Zhao Deng,Li-Hua Chen,Bao-Lian Su
Copper based catalysts have high potential for the substituent of noble-metal based catalysts as their high selectivity and moderate activity for selective hydrogenation reaction; however, achieving further high catalytic stability is very difficult. In this work, the carbonization process of Cu-based organic frameworks was explored for the synthesis of highly-dispersed Cu supported by hierarchically porous carbon with high catalytic performance for selective hydrogenation of 1,3-butadiene. The porous hierarchy of carbon support and the dispersion of copper nanoparticles can be precisely tuned by controlling the carbonization process. The resultant catalyst carbonized at 600 °C exhibits a rather low reaction temperature at 75 °C for 100% butadiene conversion with 100% selectivity to butenes , due to its reasonable porous hierarchy and highly-dispersed copper sites. More importantly, unprecedentedly stability of the corresponding Cu catalyst was firstly observed for selective 1,3-butadiene hydrogenation, with both 100% butadiene conversion and 100% butenes selectivity over 120 h of reaction at 75 °C. This study verifies that a simply control the carbonization process of metal organic frameworks can be an effective way to obtain Cu-based catalysts with superior catalytic performance for selective hydrogenation reaction.
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CHINESE JOURNAL OF CATALYSIS
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2020
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IF 6.146
Sujuan Zhang,Shixiang Duan,Gaoli Chen,Sugang Meng,Xiuzhen Zheng,You Fan,Xianliang Fu,Shifu Chen
Enhancing the separation efficiency of photogenerated carriers is propitious for the promotion of photocatalytic hydrogen production from formic acid decomposition. Herein, MoS 2 /Zn 3 In 2 S 6 (MoS 2 /ZIS6) composite photocatalysts containing varying mass percentages of MoS 2 were obtained by a straightforward synthetic method. The results confirmed that MoS 2 , as a cocatalyst, markedly promoted the photogenerated charge separation efficiency and visible light-driven hydrogen production activity of ZIS6 (λ > 400 nm). Specifically, the as-prepared 0.5% MoS 2 /ZIS6 photocatalyst exhibited the highest photocatalytic hydrogen production rate (74.25 µmol·h −1 ), which was approximately 4.3 times higher than that of ZIS6 (17.47 µmol·h−1). The excellent performance of the 0.5% MoS 2 /ZIS6 photocatalyst may be due to the fact that MoS 2 has a low Fermi energy level and can thus enrich photogenerated electrons from ZIS6, and furthermore reduce H + derived from formic acid, to form hydrogen. The structure and morphology of the MoS 2 /ZIS6 photocatalysts and the reactive species were determined by X-ray diffraction, transmission electron microscopy, and field emission scanning electron microscopy, among others; a plausible mechanistic rationale is discussed based on the results.
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NEW CARBON MATERIALS
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2026
·Vol. 41
·期 4
·917-927
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IF 7.2
Hong Zhu,Yu Cui,Qi Han,Cunhe Li,Rui Zhou,Xiaoyu Chi,Yanfeng Shen,Meijun Wang,Chunli Guo,Liping Chang
To solve the problems of limited capacity, low initial coulombic efficiency, and poor long-term cycling stability in hard carbon anodes for sodium-ion batteries, a stabilization strategy is reported that uses both microporous confinement and chemical bonding to control the sulfur species. Hard carbon is derived from bituminous coal, taking advantage of its naturally condensed aromatic framework. Using a two-step thermal process, a microporous carbon framework was constructed, followed by gasphase sulfidation to introduce sulfur species. The sulfur is confined in the micropores while forming stable covalent C-S bonds with the carbon matrix, which stabilizes the sulfur by both physical and chemical means and thus suppresses sulfur migration, which prevents interfacial side reactions and introduces additional redox-active sites. As a result, the sample delivers a high reversible capacity of 450 mAh/g after 800 cycles at a current density of 1 A/g, with excellent rate capability and cycling stability. Analysis of the storage mechanism shows that the stabilized sulfur species can reversibly participate in the sodium-ion storage and improve interfacial kinetics. Download: Download high-res image (150KB) Download: Download full-size image
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CHINESE JOURNAL OF CATALYSIS
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2023
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IF 16.5
Wen Zhang,Cai-Cai Song,Jia-Wei Wang,Shu-Ting Cai,Meng-Yu Gao,You-Xiang Feng,Tong-Bu Lu
Existing artificial photosynthesis systems often underperform due to challenges in water oxidation and extensive photogenerated carrier transfer. Herein, we demonstrate that β- cyclodextrin-decorated CdS nanocrystals (CdS-CD) can simultaneously anchor cobalt tetraphenyl porphyrin (CoTPP) catalysts and alcohol reductants onto CdS surfaces through bidirectional host-guest interactions between β- CD and CoTPP/alcohol. This configuration ensures swift electron transfer from CdS to β -CD bonded CoTPP, facilitating CO 2 reduction to HCOOH. Results showcase a remarkable yield of 1610 μmol g −1 h −1 and a 96.5% selectivity. Meanwhile, photogenerated holes in CdS are efficiently neutralized by β -CD bonded furfuryl alcohol, achieving a furfural yield of 1567 μmol g −1 h −1 and > 99% selectivity. In contrast, the discrete CoTPP-CdS system achieved a HCOOH yield of only 306 μmol g −1 h −1 and a poor HCOOH selectivity of 46.4%. It was also observed that the CoTPP@CdS-CD system maintained high CO 2 -to-HCOOH conversion rates when using other alcohols as reductants.
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CHINESE JOURNAL OF CATALYSIS
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2023
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IF 16.5
Xin Liu,Maodi Wang,Yiqi Ren,Jiali Liu,Huicong Dai,Qihua Yang
The construction of enzyme-mimicking catalysts is a crucial route for achieving green chemical transformations; however, integrating multiple sites into one catalyst is challenging. Herein, a facile method is reported to combine different active sites by constructing a modularized catalytic system. A modularized catalytic system composed of covalent organic frameworks (COFs) and Cu 2 Cr 2 O 5 exhibits remarkable efficiency in the transfer hydrogenation of cinnamaldehyde, with a selectivity of over 99% towards cinnamyl alcohol, surpassing the reaction rate of Cu 2 Cr 2 O 5 by more than fourfold. The results of the mechanistic study and density functional theory calculations suggest that the enhanced activity of the modularized catalytic system is derived from the hydrogen bonds between the COFs and isopropyl alcohol, which promote isopropyl alcohol dehydrogenation and hydride transfer. In addition, the modularized catalytic system is efficient for various saturated and unsaturated aldehydes and could be replaced by different submodules. This study demonstrates the efficiency of a modularized catalytic system for mimicking the functions of enzymes in catalysis.
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CHINESE JOURNAL OF CATALYSIS
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2023
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IF 16.5
Na Zhou,Jiazhi Wang,Ning Zhang,Zhi Wang,Hengguo Wang,Gang Huang,Di Bao,Haixia Zhong,Xinbo Zhang
Electrochemical conversion of nitrate (NO 3 − ) pollutants into chemical feedstock and fuel ammonia (NH 3 ) can contribute to sustainable mitigation of the current severe energy and environmental crises. However, the electrocatalytic NO 3 − reduction to NH 3 (NRA) involves a sluggish multielectron and proton transfer process that competes with the hydrogen evolution reaction (HER) in aqueous media, imposing great challenges in developing highly selective catalysts for NRA. In this study, we developed a copper and copper-tetracyanoquinodimethane composite catalyst (Cu@CuTCNQ), which possesses a high density of copper vacancy defects. This catalyst has been proven to be efficient for NRA through an in situ electrochemical reconstruction method. The structural evolution of CuTCNQ during NRA was investigated by in situ Raman spectroscopy, which indicated an accelerated charge transfer from the CuTCNQ substrate to the derived Cu, which facilitated the adsorption activation of NO 3 − . The obtained Cu@CuTCNQ exhibited an excellent catalytic performance for NRA, with a Faradaic efficiency of 96.4% and productivity of 144.8 μmol h −1 cm −2 at −0.6 V vs . a reversible hydrogen electrode, superior to Cu nanoparticle counterparts and most Cu-based catalysts. Cu vacancy defects and sufficient interfacial charge transfer synergistically optimize the charge distribution of Cu active sites, reduce the energy barrier for NO 3 − adsorption, and promote deoxidation and hydrogenation processes, thus enhancing NRA and selectivity.
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International Journal of Electrochemical Science
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2023
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IF 1.5
Baoyang Lu,Yao Lu,Yangping Wen,Xuemin Duan,Jingkun Xu,Shuai Chen,Long Zhang
A novel chiral L-alanine-modified 3,4-ethylenedioxythiophene (EDOT) precursor, (2S)-(2,3-dihydrothieno[3,4- b ][1,4]dioxin-2-yl)methyl 2-( tert -butoxy carbonylamino)propanoate (EDOT-Boc-Ala), was synthesized and electropolymerized in CH 2 Cl 2 –Bu 4 NBF. The corresponding polymer, poly((2S)-(2,3-dihydrothieno[3,4- b ][1,4]dioxin-2-yl)methyl 2-( tert -butoxy carbonylamino)propanoate) (PEDOT-Boc-Ala) film showed good redox activity and stability. The electrochemical behavior, structural characterization, chirality, solubility, spectroscopic properties, thermal stability, and morphology of PEDOT-Boc-Ala film were investigated. Both doped and dedoped PEDOT-Boc-Ala film could well dissolve in strong polar solvents such as dimethyl sulfoxide, tetrahydrofuran, and acetone, etc. The determination of specific rotation showed that the electropolymerization of EDOT-Boc-Ala did not influence its conformation and the polymer exhibited an enhanced specific rotation ([α] 20.0 = -191.08°) in comparison with that of the monomer ([α] 20.0 = -30.77°). Moreover, the amperometric biosensor based on PEDOT-Boc-Ala film (as immobilization matrix of biologically-active species) was successfully fabricated and employed to determine the concentration of vitamin C.
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International Journal of Electrochemical Science
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2023
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IF 1.5
Jingyi Chen,Chao Zhou,Hongyu Liu,Ping Li,Yonghai Song,Fugang Xu
A self-powered electrochemical sensor (SPS) has been designed for sensitive detection of glucose based on the glucose oxidase (GOD)/polyvinyl ferrocene (PVF)/ poly(diallyldimethylammonium chloride) (PDDA -reduced graphene oxide (RGO)/glassy carbon electrode (GCE) as a bioanode and bilirubin oxidase (BOD)/PDDA-RGO/GCE as a biocathode. The signal amplification of electron mediator in the electrochemical anode has been investigated in details. The results exhibited that the electron mediator did amply the signal of SPS and the mediator existed on the surface of electrode was better than that existed in a solution. The electrodes constructed under the optimal conditions have 2 been used to develop a glucose SPS which showed a wide linear range from 0.1 mM to10 mM (R 2 =0.997) and a low detection limit of 23.7 μM (S/N=3). Therefore, the newly developed SPS was sensitive and facile for glucose detection, which could promise the possibility of its application in real samples.
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International Journal of Electrochemical Science
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2023
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IF 1.5
Qing ZHOU,Ning Long,Lan LIU,Haiyun ZHAI,Mingfang ZHU
A highly selective molecularly imprinted polymer modified carbon paste electrode was developed. The Moxifloxacin Hydrochloride molecularly imprinted polymer was synthesized by thermal initiation precipitation polymerization, and the modified electrode was prepared by mixing graphite and polymer (90:10). Studied the electrochemical behavior and established the determination method of Moxifloxacin Hydrochloride at the electrode. The results showed that the sensor has high selectivity and sensitivity. and exhibited a linear voltammetric response for Moxifloxacin Hydrochloride in the concentration range of 3.13×10 -6 ~2.0×10 -4 mol•L -1 , with the limit of detection (LOD) of 5.9×10 -8 mol•L -1 (S/N=3). The sensor was applied to determine Moxifloxacin Hydrochloride in Avelox tablets and and human serum samples. The recoveries of Moxifloxacin Hydrochloride ranged from 97.2% to 104.5%.
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