Arabian Journal of Chemistry
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2022
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IF 6.212
Jie Zhao,Yan Gong
RNA plays a crucial role in biochemical processes. RNAs with abasic sites (AP-RNA), as one of RNA lesions, will cause serious negative consequences. Efficient and sensitive detection of AP-RNA deserves but does not receive enough attention. Water-soluble uridine triphosphate (UTP)-capped Mn-doped ZnS quantum dots (QDs), which have excellent room-temperature phosphorescence (RTP) properties, were prepared by wet-chemical method. The UTP on the surface of QDs could form a precipitation complex with amiloride (AMI) to quench the RTP. Meanwhile, abasic double-stranded RNA (AP-dsRNA) with a high affinity to AMI could dissociate AMI from the surface of UTP-QDs, resulting in RTP recovery. In this process, a highly sensitive and selective RTP-detection system for AP-dsRNA was constructed with AMI as the modulation factor and UTP-QDs as the luminescence matrix. RTP was turned off and on for the determination of AP-dsRNA, and the interference of background fluorescence and scattered light was effectively avoided during complex formation and aggregation. Steric hindrance of the conformation of AP-dsRNA provided efficient selectivity. The detection limit for AP-dsRNA was 0.86 nM, the relative standard deviation was 2.1%, and the recovery of biological samples with AP-dsRNA addition ranged from 95% to 103% at optimal conditions. The system is expected to provide new methods for environmental monitoring, early disease screening, and evaluation of gene editing efficiency.
研究领域:
生物化学
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分子生物学
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分析化学
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 8
·2588-2597
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IF 9.48
Xintong Meng,Zengyong Li,Di Li,Yiming Huang,Jiaojiao Ma,Chuanfu Liu,Xinwen Peng
Catalytic and selective oxidation of monosaccharides into value-added sugar acids is highly desirable from both scientific and industrial perspectives. Here, we report a hierarchical porous carbon (NC-3) supported gold catalyst (Au/NC-3) and its application in the base-free aerobic oxidation of D-glucose and D-xylose into value-added sugar acids under mild conditions (100 °C). The catalyst exhibited excellent catalytic performance with the yields of D-gluconic acid and D-xylonic acid reaching 97.62% and 98.76%, respectively. We studied the effect of the ball-milling process on the hierarchical porous preparation, which is critical to the formation of the fibrous structure during the pyrosis process. This specific structure provides active sites for Au adsorption. DFT calculation revealed that the Au NPs prefer to anchor on pyridinic N sites; meanwhile, the initial reactants and essential intermediates are found to be well stabilized by Au/NC-3. Moreover, upon recycling, gold was stable toward the recovery procedure. In this work, we provide a green method for an improved generally selective oxidation of D-glucose and D-xylose using Au/NC-3 as an efficient heterogeneous catalyst.
研究领域:
化学
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催化科学
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DOI
高影响因子
Catalysts
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2023
·Vol. 13
·期 4
·663
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IF 3.9
Xu Wu,Heqin Guo,Litao Jia,Yong Xiao,Bo Hou,Debao Li
The base-free oxidation of furfural by non-noble metal systems has been challenging. Although MnO2emerges as a potential catalyst application in base-free conditions, its catalytic efficiency still needs to be improved. The crystalline form of MnO2is an important factor affecting the oxidation ability of furfural. For this reason, four crystalline forms of MnO2(α, β, γ, and δ-MnO2) were selected. Their oxidation performance and surface functional groups were analyzed and compared in detail. Only δ-MnO2exhibited excellent activity, achieving 99.04% furfural conversion and 100% Propo.FA(Only furoic acid was detected by HPLC in the product) under base-free conditions, while the furfural conversion of α, β, and γ-MnO2was below 10%. Characterization by XPS, IR, O2-TPD and other means revealed that δ-MnO2has the most abundant active oxygen species and surface hydroxyl groups, which are responsible for the best performance of δ-MnO2. This work achieves the green and efficient oxidation of furfural to furoic acid over non-noble metal catalysts.Keywords:base-free;MnO2;crystal type;furfural oxidation to furoic acid
研究领域:
催化化学
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绿色化学
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产品关联
DOI
高影响因子
Chemistry-Switzerland
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2023
·Vol. 5
·期 3
·1497-1507
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IF 2.1
Longlong Gao,Rui Tian,Yong Shao
DNAzymes have attracted increasing interest in developments of gene tools, therapies, and biosensors. Among them, G-quadruplexes are widely used as the key structure elements of DNAzymes to activate the catalytic competency of specific cofactors, such as hemin, but there is a great demand to diversify DNAzymes using other more straightforward DNA structures such as fully matched duplex (FM-DNA). However, the perfect base pairs in duplex limit the DNAzyme activity. In this work, a photocatalytic DNAzyme was developed by introducing an abasic site (AP site) into duplex (AP-DNA) to switch its photocatalytic activity. Palmatine (PAL), a photosensitizer from natural isoquinoline alkaloids, served as a cofactor of the DNAzyme by binding at the AP site. The AP site provides a less polarized environment to favor the PAL fluorescence. As a result, dissolved oxygen was converted into singlet oxygen (1O2) via energy transfer from the excited PAL. The oxidation of substrates by the in situ photogenerated1O2served as a readout for the DNAzyme. In addition, the duplex-based DNAzyme was engineered from FM-DNA by the cascade uracil-DNA glycosylase to generate AP-DNA. Our work provides a new way to construct duplex-based DNAzymes.Keywords:DNAzyme;duplex;abasic site;phohocatalysis;isoquinoline alkaloids;palmatine
研究领域:
生物化学
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分子生物学
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催化
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
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2022
·Vol. 24
·期 22
·8840-8852
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IF 11.034
Zongyang Liu,Yuan Tan,Jie Li,Xiuli Li,Yan Xiao,Juan Su,Xingkun Chen,Botao Qiao,Yunjie Ding
Aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is a promising alternative route to produce renewable biodegradable plastics, which has stimulated intense interest in recent years. Supported gold catalysts have shown great potential for this reaction, but the selectivity and stability need to be improved. In addition, the requirement for base additives makes the process less effective and sustainable. Herein, highly active and selective Au–Ag bimetallic nanoclusters supported on MgAl-hydrotalcite (HT) were developed for HMF oxidation to FDCA under base-free reaction conditions using molecular oxygen as the oxidant. The presence of small amounts of Ag (0.034–0.065 wt%) in Au25 clusters greatly enhanced the catalytic reaction rates and selectivity for HMF tandem oxidative steps, leading to both high conversion of HMF (>97%) and high yield of FDCA (>95%). Besides, the catalyst stability was also enhanced by the addition of Ag. The characterization results suggested that the substitution of Ag atoms modified the electronic structure of Au while likely maintaining the primary geometry. Thus, a significant synergistic effect could be observed over trace Ag modified Au–Ag bimetallic nanoclusters. The present work provides new insight into the alloying effect, and helps understand highly efficient Au-based catalysts for aerobic oxidation of biomass derived molecules under base-free conditions.
研究领域:
催化化学
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可再生资源化学
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DOI
高影响因子
CARBOHYDRATE RESEARCH
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2024
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IF 2.4
Xiao Du,Tengfei Li,Lumei Wang,Dezhang Ren,Zhibao Huo
In recent years, the research on the conversion of chitin to high value-added chemicals has attracted more and more attention. At present, the method of preparing lactic acid from chitin mostly uses strong base or catalyst. The reaction system under alkaline condition not only corrodes the container but also easily harms the human body. Herein, a simple and effective method to convert chitin to organic acids in catalyst and base-free conditions is developed. The use of H 2 O 2 only can efficiently convert chitin to organic acids in the absence of bases and catalysts. Under the optimal conditions of 30 mg chitin, 2.1 mL water, 0.9 mL H 2 O 2 at 230 °C for 1.5 h, the lactic acid yield of chitin can reach 58.2 % and the total organic acid yield can reach 84.0 %. This work provides an efficient method for the resource utilization of chitin biomass.
研究领域:
生物化学
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生物质能
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绿色化学
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DOI
高影响因子
GREEN CHEMISTRY
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2023
·Vol. 25
·期 3
·1179-1190
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IF 9.8
Yaohong Zhou,Wanming Xiong,Yujing Jin,Peng Wang,Weiqi Wei,Jiliang Ma,Xiaohua Zhang
Conversion of lignin feedstocks into aromatic chemicals is a highly desirable target for biorefineries, and their depolymerization often requires high temperatures and harsh conditions. In this work, a process optimization involving several factors, including catalyst dosage, reaction temperature, reaction time, oxygen pressure and solvent effect, towards vanillin production from the oxidation of lignin-based vanillyl alcohol in a base-free solvent over a LaFeO3 perovskite was proposed. The results pronounced that the LaFeO3 perovskite exhibited excellent catalytic performance for affording a 100.0% conversion rate of vanillyl alcohol and 33.0% vanillin yield with the addition of 0.1 g LaFeO3 dosage at 180 °C for 2 h under 1.0 MPa O2 supply in ethyl acetate solvent. Furthermore, the presence of oxygen vacancies (Fe3+–□–Fe2+) in the LaFeO3 perovskite contributed to combining with molecular oxygen to generate the active species [Fe3+O2−], which played a key role in the oxidation of vanillyl alcohol and dominated the formation pathway of vanillin. On the other hand, reusability tests manifested that the performance of LaFeO3 decreased gradually with the increase of consecutive runs and was strongly negatively related to the amount of carbon deposits, as carbon deposits would prevent vanillyl alcohol from being accessible to active sites. Nevertheless, the performance of the spent LaFeO3 catalyst could be easily regenerated by a simple calcination approach. Overall, this work provides the possibility of a scalable strategy for constructing LaFeO3-based perovskites as efficient and reusable catalysts for vanillin production from biorefinery lignin.
研究领域:
化学工程
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生物炼制
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催化材料
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产品关联
DOI
高影响因子
CEMENT AND CONCRETE RESEARCH
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2025
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IF 13.1
Xin Liu,Dining Li,Mingqi Li,Hui Xie,Xiaohan Yu,Haochuan Wang,Wei Wang,Jinxiang Hong,Zuhua Zhang,Pan Feng
Magnesium salts are key components of liquid alkali-free accelerator; however, their influence on the setting and hardening of accelerated cement pastes remains unclear. This study systematically investigates the role of different magnesium salts by preparing and examining aluminum sulfate (AS)-based accelerators at different dosages. The effects of the accelerators on the setting and early age mechanical properties of the cement pastes were comparatively studied. Results revealed that the type and dosage of magnesium salts significantly affected these properties. Specifically, MgSiF 6 substantially accelerated the cement paste setting, albeit at the expense of early age mechanical strength, owing to its considerable delay in C 3 S hydration. Conversely, both Mg(NO 3 ) 2 and MgSO 4 slightly shortened the setting time while improving the 6 h compressive strength, which was attributed to the facilitation of C 3 S hydration and refinement of the cement pore structure. Further analysis of ettringite formation, growth and chemical composition indicated that the low pH environment induced by MgSiF 6 promoted the incorporation of magnesium and fluoride ions into ettringite, leading to the formation of higher-aspect-ratio crystals. This morphological change enhanced the percolation network, thus accelerating cement setting. These findings advance our understanding of the setting and hardening mechanisms of accelerated cement pastes and offer valuable guidelines for optimizing accelerator formulations.
研究领域:
材料科学
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土木工程
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产品关联
DOI
高影响因子
ChemSusChem
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2022
·Vol. 15
·期 16
·e202201041
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IF 9.14
Wen Guan,Yunlei Zhang,Changhao Yan,Yao Chen,Yanan Wei,Yu Cao,Fang Wang,Pengwei Huo
Graphical Take a bow ( l ): Benefiting from the alloying effect for supported bimetallic AuPd catalyst and the formation of hydroxyl radical initiated by H 2 O dissociation on hydrophilic surface, base-free aerobic oxidation of furfuralcohols and furfurals to furancarboxylic acids is performed over AuPd/pBNC- x %HNO 3 bowl-like catalysts. Upgrading furfuralcohols and furfurals to furancarboxylic acids is of great significance for high value-added downstream chemicals synthesis and biomass conversion. Developing an efficient catalyst is the key to acquiring a completely sustainable process. Herein, nitrogen-doped carbon-supported bimetallic AuPd bowl-like catalysts were synthesized. The surface wettability of nitrogen-doped carbon was well adjusted by the nitrification process. Benefiting from the alloying effect of bimetallic AuPd catalyst and the formation of hydroxyl radical initiated by H 2 O dissociation on the hydrophilic surface of nitrated nitrogen-doped carbon, base-free aerobic oxidation of 5-hydroxymethylfurfural (HMF) could produce the highest 2,5-furandicarboxylic acid (FDCA) yield of 93.9 %. In-situ infrared spectroscopy uncovered adsorption configuration of HMF, and the nitrated carbon surface was favorable for HMF and intermediates to enter the active sites, greatly promoting the catalytic oxidation process. Employing other furfuralcohols (furfuryl alcohol, furan-2,5-diyldimethanol, 2,5-bishydroxymethylfuran) as well as furfural and 5-methylfurfural as starting materials, 35.6–95.4 % yield of furancarboxylic acids (FDCA, 2-furoic acid, 5-methyl-2-furoic acid) were also obtained. Moreover, the developed catalysts could maintain excellent stability and activity after four successive runs. This deep insight into the role of bimetallic synergy and surface wettability provides a basis for the rational design of the highly efficient catalysts for the oxidation of furfuralcohols and furfurals and related reactions.
研究领域:
催化化学
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生物质转化
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绿色化学
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DOI
高影响因子
Green Processing and Synthesis
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2022
·Vol. 11
·期 1
·823-829
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IF 3.97
Bo Jiang,Yue-Yue Du,Guo-Zhi Han
Herein, we report a new one-step direct synthesis of aromatic azo compounds from anilines under mild conditions. With the catalysis of copper acetate mediated by palladium salt, rapid conversion of anilines to aromatic azo compounds can be observed under the conditions of base-free along with solvent-free. Furthermore, the cross-coupling nitridation reaction based on this strategy was also studied. This research provides not only a new way for the synthesis of symmetrical and asymmetrical aromatic azo compounds but also a strategy and platform for exploring catalytic applications of transition metal compounds.
研究领域:
有机化学
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催化化学
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DOI
高影响因子
Molecular Catalysis
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2023
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IF 4.6
Jie Huang,Wenhao Yang,Sen Zhang,Jingjie Luo,Changhai Liang
Catalytic hydrogenation of adiponitrile to hexamethylenediamine (HMDA) via alkali-free processes is essential to produce high-value downstream chemicals. In this work, we synthesized a series of Co@C CNT x catalysts using CNT promotion to strength the carbon skeleton derived by ZIF-67. Compared to the Co@C without CNT promotion, great enhancement of HMDA yield was achieved by Co@C CNT x . Characterizations suggested that CNT in the precursor modified the crystallization of the active Co centers as well as the surface composition in the Co@C CNT x . Strong Co-carbon interaction was formed via Co-N coordination caused by the facilitated re-dispersion of N- containing functionalities. The ethanol contact angle on Co@C CNT x was changed for better mass transfer and diffusion of reaction liquid on the catalyst. As a final result, the oxidation of cobalt sites was greatly suppressed in Co@C CNT 0.3 and Co@C CNT 0.5 , which was proved an essential factor for their fast reaction rates. 88 % yield of HMDA with the rate of 4.5 mol HMDA /mol Co /h was reached under a much higher utilization rate of Co center.
研究领域:
化学工程
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催化化学
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产品关联
DOI
高影响因子
LANGMUIR
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2024
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IF 3.7
Zixin Zhong,Yingdan Ye,Yibin Zhang,Weichen Du,Zhaoyin Hou
Polylactic acid (PLA) plastics are the most popular biodegradable and biocompatible materials; however, their monomer, lactic acid (LA), is currently produced via an inefficient fermentation process. Herein, activated carbon-supported Pt–Cu intermetallic compounds were synthesized and utilized in the selective oxidation of 1,2-propanediol (1,2-PDO) toward LA without the participation of homogeneous alkali or a basic support. It was found that rhombohedral intermetallic Cu1Pt compounds exhibited excellent performance and the calculated turnover frequency of each surface Pt atom reached 10 049 h–1. The yield of free LA reached 64.6% with a complete conversion of 1,2-PDO at 100 °C within 2 h. Diverse characterization and DFT calculations revealed that Pt–Cu intermetallic compounds were active for the adsorption and/or activation of molecular oxygen and 1,2-PDO. Raman analysis of adsorbed 1,2-PDO further disclosed that 1,2-PDO contacted with rhombohedral intermetallic Cu1Pt compounds strongly, and then the oxidation of the terminal hydroxyl group was performed preferentially, which promoted the formation of LA.
研究领域:
化学工程
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材料科学
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催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）