BIOSENSORS & BIOELECTRONICS
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2017
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IF 7.78
Wenjing Jiang,Linni Wu,Junling Duan,Huanshun Yin,Shiyun Ai
An ultrasensitive sandwiched electrochemiluminescence (ECL) immunosensor was developed for 5-hydroxymethylcytosine (5hmC) detection in genomic DNA by using Fe 3 O 4 @SiO 2 core–shell magnetic nanomaterial as a immobilization matrix for anti-5hmC antibody, PAMAM conjugated avidin and Ru(bpy) 2 (phen-5-NH 2 )(PF 6 ) 2 as signal amplification unit. Importantly, Fe 3 O 4 @SiO 2 nanoparticles were verified to not only possess enormous surface for loading antibody by amido link, but also exhibit excellent bioactivity . With the dual signal amplification strategy, the ECL immunosensor showed wide detection range from 0.1 to 30 nM with low detection limit of 0.047 nM (S/N = 3). Based on the specific immunoreaction, the developed method also illustrated excellent detection selectivity . The fabricated immunosensor was also applied to detect the 5hmC in genomic DNA of cancer tissue, which indicated that the immunosensor possess potential applications in clinical detection.
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INORGANIC CHEMISTRY
·
2024
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IF 4.3
Hongliang Dai,Pengjie Zhou,Shenming Yang,Lili Yang,Hongye Bai,Cui Dai,Guohai Xu,Weiqiang Fan
Electrocatalytic conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is significant for the sustainable production of value-added chemicals. Active sites of catalysts could enhance the activity and selectivity of the HMF oxidation reaction (HMFOR), but the self-healing ability of active sites has been commonly ignored. In this work, Co(OH)2/Ni-MOF was successfully fabricated for efficient oxidation of HMF to FDCA under mild conditions. Electrochemical and cyclic stability experiments demonstrated the high self-healing properties of the dual active sites (Co3+/Ni3+). So, the retention rate of FDCA yield can still reach 98.5%, even after 90 days. HMFOR was further coupled with 4-nitrophenol hydrogenation, which promotes the yield and Faradaic efficiency of FDCA to about 100%. Therefore, this study explores the self-healing properties of species and provides new insights for designing efficient catalysts.
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Russian Journal of Physical Chemistry A
·
2024
·Vol. 98
·期 8
·1740-1751
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IF 0.7
Yanliang Zhai,Lu Xianggang,Zhang Wanli,Chen Hao,Li Gaolong,Zhang Jian,Li Zhijun,Wang Jun
Abstract— Cr- and Pt-based catalysts are the most widely used industrial catalysts for propane dehydrogenation (PDH). However, these catalysts still show disadvantages such as environmental toxicity and high economic cost. Cobalt (Co)-based catalysts have become promising candidate catalysts for PDH reactions due to their environmental friendliness and low cost. In this paper, Co-based catalysts are prepared by the impregnation method and precipitation method, respectively. The obtained catalysts all show grape-like nanocrystalline aggregated structures with intercrystallite mesopores and high surface area. This can improve the dispersion of Co species and mass transfer of catalysts. Comparing catalysts prepared by the two methods, the impregnated 1CoZI sample shows smaller CoO x nanoparticle size and higher Co 2+ /Co 3+ ratio than the precipitated 1CoZP sample. Moreover, the impregnated 1CoZI sample shows higher propane conversion and propylene selectivity, which is attributed to the smaller CoO x nanoparticle size and higher content of Co 2+ species bonded with zeolite framework. This structure brings higher catalytic activity and stability to the catalyst. Different PDH reaction conditions such as the reaction temperature and propane GHSV are also investigated. Under the optimal PDH reaction conditions (525°C and 4500 h –1 ), the impregnated 1CoZI shows high propane conversion (32%) and propylene selectivity (86%).
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FUEL
·
2025
·
IF 7.5
Yan Tan,Xiao Liu,Yujia Zhang,Yiyang Rong,Xueying Wu,Ting Liu,Zizhen Ma,Huawei Zhang
In the current study, catalytic oxidation technology is among the most widely used methods for removing chlorinated volatile organic compounds (CVOCs). This article details the preparation of the Ag-Mn@ZSM-5 catalyst, which was prepared via the hydrothermal approach, followed by the incorporation of nano-Ag. The focus of the study is the catalytic oxidation of chlorobenzene (CB). Experimental results indicate that the hydrothermally synthesized nano-silver modified Ag-Mn@ZSM-5 catalyst, exhibiting a T90 of 290 °C, demonstrates superior performance compared to the Ag-Mn/ZSM-5 catalyst prepared via the traditional impregnation method, which has a T90 of 365 °C. As the operating airspeed increased from 7000 h −1 to 42000 h −1 , the removal efficiency of CB consistently remained above 90%, with stability maintained over a duration of 30 h. Furthermore, the catalyst exhibited excellent water resistance during a 12 h switching water test. Based on the characterization results, after loading Ag, the ratio of Mn 4+ and Mn 3+ on the surface of the Ag-Mn@ZSM-5 catalyst increases, the reducibility is enhanced, and the surface adsorbed oxygen species is increased, which is conducive to improving the catalytic activity. In addition, the Ag-Mn@ZSM-5 catalyst possesses an optimal pore structure, the proportion of mesoporous is 79.06%, suitable redox capacity, abundant acidic sites, and features a compact crystal stacking structure, which results in remarkable stability, catalytic activity, and space velocity resistance of the catalyst. These advantageous properties facilitate the adsorption and deep oxidation of CB. This study presents promising prospects for industrial applications and aims to offer innovative strategies for the treatment of chlorine-containing waste gases.
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FUEL
·
2024
·
IF 6.7
Zekun Guan,Guangxun Sun,Chao Feng,Junxi Li,Minmin Wang,Mengdi Guo,Bin Liu,Yuan Pan,Chenguang Liu,Yongming Chai,Yunqi Liu
The production of cleaner gasoline requires reducing sulfur and olefin content in fluid catalytic cracking (FCC) gasoline. Herein, Ni/ZSM-5@Ni/ZnO catalysts were synthesized by uniformly coating Ni/ZnO on the surface of Ni/ZSM-5 by electrostatic induced crystallization strategy for FCC gasoline desulfurization-aromatization tandem reactions. The desulfurization activity of Ni/ZSM-5@Ni/ZnO has superior desulfurization activity due to the smaller size of ZnO, higher O vacancy content, and more uniform dispersion of Ni and ZnO relative to the physically mixed Ni/ZSM-5-Ni/ZnO. In addition, coating Ni/ZnO on the surface of Ni/ZSM-5 can reduce the Brønsted acid content of Ni/ZSM-5, increase the Lewis/Brønsted acid value of the catalyst, which inhibits the excessive cracking of FCC gasoline, and improves the liquid yield and aromatics selectivity. After 8 h of reaction, the desulfurization rate, aromatics generation rate and olefin conversion rate of Ni/ZSM-5@Ni/ZnO were 85.58 %, 25.22 % and 49.08 % respectively, which were higher than those of physically mixed Ni/ZSM-5-Ni/ZnO catalysts by 25.34 %, 15.95, and 12.98 %, respectively. Meanwhile, the unique structure of Ni/ZSM-5@Ni/ZnO reduces carbon deposition and delays catalyst deactivation. Density functional theory calculations show that Ni/ZSM-5@Ni/ZnO was more favorable for thiophene desulfurization and has a better ability to adsorb and activate H 2 . This study provides a new idea for the development of catalysts for clean gasoline production.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Hongyu Qu,Xiangcheng Li,Xiao Han,Junjie Li,Xinqiang Feng,Chuang Liu,Zhendong Wang,Weimin Yang
Rational design of highly efficient non-noble-metal catalysts for the selective hydrogenolysis of biomass platform compounds to produce fuels and fine chemicals is a key pursuit for the sustainable chemical industry. In this work, we report for the first time the synthesis of a Ni-supported germanosilicate zeolite (Ni-SCM-14) catalyst by a simple grinding method, showing both satisfactory yield (90.3%) and good stability in eight cycles for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF). Characterization revealed that Ni nanoparticles were highly dispersed on the SCM-14 zeolite with strong interactions. The synergistic effect of highly dispersed Ni hydrogenation sites and the weak acidity activation of the C–O bond provided by SCM-14 is considered to be the key to the efficient hydrogenolysis of HMF. This discovery opens up a new avenue for germanosilicate zeolite to activate the C–O bond.
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CATALYSIS TODAY
·
2024
·
IF 5.2
Chengfeng Yi,Jingwen Li,Zhigang Liu
NiS X stands out in the electrochemical oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) due to the favorable conductivity and diverse chemical composition. However, NiS X usually exhibits few exposed active sites and poor charge transfer kinetics. Moreover, during the electrochemical oxidation of HMF, the conductivity of the catalyst would decrease rapidly with the formation of oxidized Ni species, leading to a rapid decline in catalytic performance. Therefore, a series of NiS X /carbon black (CB) hybrids (NiS X /CB-n) were synthesized via a one-step solvent hydrothermal method in which NiS X displayed a large cubic block structure assembled from small nanosheets. Among the prepared catalysts, NiS X /CB-2, with the optimal amount of introduced CB, exhibited superior electrocatalytic activity for the oxidation of HMF, achieving 100% HMF conversion, 98% FDCA yield, and 100% Faradaic efficiency at 1.45 V (vs. RHE). The outstanding electrocatalytic activity of NiS X /CB-2 was attributed to the suitable CB doping, which not only enhanced the conductivity of catalyst but also separated the small nanosheets, preventing the formation of densely packed NiS X structure and increasing the specific surface area of catalyst, thereby exposing more active sites and improving the availability of material. Furthermore, the formation of C-S bonds facilitated charge interactions between NiS X and CB, promoting the transfer of charges during the electrolysis process and enhancing electrocatalytic kinetics. Open circuit potential tests demonstrated that the introduction of CB also strengthened the adsorption capacity of catalyst for HMF, further benefiting its electrocatalytic activity.
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PROCESS BIOCHEMISTRY
·
2024
·
IF 3.7
Fanjin Meng,Qian Zheng,Yuqiu Wu,Lishi Yan,Zhi Chen,Xin Ju,Liangzhi Li
The enzymes used for D-allose production generally failed to meet the requirements of industrial production of D-allose in terms of enzyme activity and catalytic efficiency. In this study, 13 single mutants of CfRpiB (Ribose-5-phosphate isomerase from Curtobacterium flaccumfaciens ) were constructed by combining site-specific mutations and ring-open residue mutations with rational design. It was found that the enzyme activities of all 13 single mutants were positively changed relative to the wild type. Among them, the single mutant with the highest increase in enzyme activity was C72M, which increased its enzyme activity by 30 %. On this basis, three iterative mutant strains were constructed, among which C72M/S105H increased the yield of D-allose by 2.62 times. Especially, enzymatic property measurements showed that its enzyme activity increased by 50 %. Molecular docking of the C72M/S105H mutant with D-allulose revealed that the increased enzymatic activity of the mutant C72M/S105H could be attributed to the smaller substrate binding site and tighter binding to the substrate. This study further reveals the relationship between mutation sites and enzymatic properties, demonstrating the feasibility of improving the efficiency of preparing rare sugars through enzyme molecular modification.
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REACTIVE & FUNCTIONAL POLYMERS
·
2024
·
IF 4.5
Linlin Yu,Ruoyu Chen,Qian Jia
Oily wastewater, especially oil-water emulsions, has caused severe environmental damage. It is urgent to develop a simple, efficient superhydrophobic and superoleophilic material to address this issue. In this work, a multifunctional sponge based on MOF was proposed. The hydroxy-assisted method was employed to prepare MOF-5 with metal coordination centers. Subsequently, octadecylphosphonic acid (OPA) was used to hydrophobically modify MOF-5 to prepare stable and hydrophobic OPA-MOF-5. Polydimethylsiloxane (PDMS) with low surface energy was employed as the adhesive, and the hydrophobic OPA-MOF-5 was loaded onto the polyurethane (PU) sponge to obtain the stable superhydrophobic OPA-MOF-5@PDMS@PU with a WCA of 155.9°. The produced modified sponge exhibited high sorption capacity and oil-water separation efficiency, with a sorption capacity of 26.7 (petroleum ether)-85.6 (chloroform) g/g and a separation efficiency of over 99 %. It has also shown satisfactory emulsion purification and flame retardancy capacities.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2024
·
IF 2.8
Haoyu Liu,Jingye Ma,Hong Yuan,Xiang Shi
BACKGROUND A series of Pt@NZSM–5 and Pt/NZSM–5 nanosheets having different Si/Al ratios were prepared via an in situ synthesis and impregnation method, respectively, using C 22 H 45 –N + (CH 3 ) 2 –C 6 H 12 –N + (CH 3 ) 2 –C 6 H 13 (C 22–6–6 ) as the template agent. The oleic acid decarboxylation reaction was carried out using these materials under CO 2 atmosphere and the oleic acid cracking mechanism was inferred from the product distribution of the C8-C17 alkanes. RESULTS The Pt@NZSM–5 and Pt/NZSM–5 was found to comprise thinner nanosheets and exhibited strong metal–substrate interactions. Pt@NZSM–5 nanosheets with a Si/Al molar ratio of 100 had thicknesses of only 8–9 nm along with a mesopore/micropore capacity ratio of 2.7, an acid content of 11 cm 3 /g STP and a high Pt 0 /PtO x ratio. CONCLUSION The Pt@NZSM-5 and Pt/NZSM-5 nanosheets had an interconnected hierarchical system and a large number of metal active sites that facilitated the decarboxylation of oleic acid. The Pt@NZSM–5 nanosheets demonstrated excellent catalytic activity during the cracking of oleic acid under a CO 2 atmosphere, giving a yield of C8–C17 alkanes as high as 83.8% after 5 h at 320 °C. These Pt@NZSM–5 nanosheets also showed greater stability than the Pt/NZSM–5 specimens. © 2024 Society of Chemical Industry (SCI).
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Hongwei Zhang,Hao Xu,Zhen Zhu,Jinming Huang,Bowen Zhang,Yafei Cheng,Xiaocheng Lin,Bin Wu
The electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) represents a promising pathway for producing biomass-derived value-added chemicals. Nevertheless, the use of extremely expensive ion exchange membranes (IEMs) as separators significantly sacrifices the economic benefit in large-scale applications. Herein, we report a cost-effective non-fluorine cation exchange membrane (CEM) by grafting sulfonic acid (-SO 3 - ) groups onto the aromatic side chain of the polyethersulfone (PES) polymer. By tuning the content of –SO 3 - groups, the physicochemical properties of the resulting CEMs can be easily adjusted. Impressively, the optimal HBS-PES-1.0 CEM with fully grafted –SO 3 - groups can achieve a high HMF conversion of 100 %, FDCA selectivity of 98.0 %, and Faradaic efficiency of 98.3 % when used as the separator for electrocatalytic oxidation of HMF, surpassing that of the commercial Nafion 117 membrane (100 % HMF conversion, 98.1 % FDCA selectivity, and 97.4 % Faradaic efficiency). This study provides a cost-effective and high-performance CEM as a substitute for the expensive commercial membrane, paving the way to large-scale commercial applications of biomass upgrading through the electrolysis process.
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iScience
·
2024
·
IF 4.6
Junfu Zhou,Yuting Miao,Hongxin Ding,Yuanhang Ren,Lin Ye,Bin Yue,Heyong He
Direct and stable conversion of CO 2 to aromatics (CTA) is an attractive route for reducing CO 2 emissions. However, due to the chemical inertness of CO 2 , direct CTA reaction with high aromatics selectivity is still challenging. In this work, a tandem catalyst Zn 0.1 Ti 0.9 O x /HZSM-5 with appropriate density and strength of acid sites exhibits a high aromatics selectivity of 67.2% and long-term stability over 100 h. Furthermore, the total selectivity of benzene, toluene, and xylene achieves 24.1% over Zn 0.1 Ti 0.9 O x /HZSM-5 with a modified hydrophilic surface. In addition, the CTA via the formate route has been determined in this reaction system.
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