Small
·
2021
·Vol. 18
·期 4
·2105696
·
IF 13.281
Qiming Chen,Ning Gong,Tanrui Zhu,Changyu Yang,Wenchao Peng,Yang Li,Fengbao Zhang,Xiaobin Fan
The oxygen evolution reaction (OER) plays a key role in many electrochemical energy conversion systems, but it is a kinetically sluggish reaction and requires a large overpotential to deliver appreciable current, especially for the non-noble metal electrocatalysts. In this study, the authors report a surface phase engineering strategy to improve the OER performance of transition metal nitrides (TMNs). The iron-nickel nitrides/alloy nanospheres (FeNi 3 -N) wrapped in carbon are synthesized, and the optimized FeNi 3 -N catalyst displays dual-phase nitrides on the surface induced by atom migration phenomenon, resulting from the different migration rates of metal atoms during the nitridation process. It shows excellent OER performance in alkaline media with an overpotential of 222 mV at 10 mA cm −2 , a small Tafel slope of 41.53 mV dec −1 , and long-term durability under high current density (>0.5 A cm −2 ) for at least 36 h. Density functional theory (DFT) calculations further reveal that the dual-phase nitrides are favorable to decrease the energy barrier, modulate the d-band center to balance the absorption and desorption of the intermediates, and thus promote the OER electrochemical performance. This strategy may shed light on designing OER and other catalysts based on surface phase engineering.
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POLYMER DEGRADATION AND STABILITY
·
2020
·
IF 4.032
Qianyu Sun,Jie Sheng,Rendang Yang
Controllable degradation is important for the biodegradable polymers used as drug carriers, because the drug release rate can be regulated by the degradation rate. Here, we synthesized chitosan-graft-poly(D, L-lactic acid) copolymers (CgPCs) with high MS PDLLA (molar substitution of poly(D, L-lactic acid)), which possessed controllable biodegradability for regulating the drug release rate. CgPCs with high MS PDLLA were prepared efficiently through an eco-friendly system of 1-ethy-3-methyimidazolium acetate (EmimAc)/4-Dimethylaminopyridine (DMAP). The MS PDLLA reached the maximum of 12.00 within 5 hours, which involved 2.91 of DS PDLLA (the degree of substitution of poly(D, L-lactic acid)) and 4.13 of DP PDLLA (the degree of polymerization of poly(D, L-lactic acid)). Importantly, the biodegradation rate of CgPCs could be regulated by the MS PDLLA . CgPCs with MS PDLLA of 3.98 showed good hydrophilicity and fast degradation leading to burst release of curcumin, whereas CgPCs with MS PDLLA of 12.00 exhibited relatively poor hydrophilicity and slower degradation resulting in sustained release of curcumin. This study provides some new possibilities for controllable biodegradation of drug carriers and optionality of burst or sustained drug release.
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PROCESS BIOCHEMISTRY
·
2019
·
IF 2.883
Ping Zhu,Yan Zeng,Peng Chen,Yan Men,Jiangang Yang,Xiaoping Yue,Jiangang Zhang,Yueming Zhu,Yuanxia Sun
A one-pot two-enzyme reaction system was developed to produce high-fructose syrup (HFS) containing healthy rare sugar d-allulose from Jerusalem artichoke (JA). Inulin in JA was converted through the cascade reaction of a novel exo-inulinase from Bacillus velezensis (BvInu) and D-allulose 3-epimerase from Ruminococcu s sp. (RDAE). BvInu and RDAE were expressed in Bacillus subtilis and successfully secreted into the supernatant, which decrease the production cost and avoid enzyme purification. The optimal temperature and stability of extracellular BvInu significantly increased, thereby promoting the catalytic activity of the two enzymes for the cascade reaction in one pot. Inulin in JA powder was almost completely converted into monosaccharides in the treatment with the optimal ratio of BvInu : RDAE (80 : 40 U/g inulin) at 50 °C for 2 h. The ratio of D-glucose, D-fructose, and D-allulose in the product was approximately 1:3:1, and the yield on JA powder was 67%. The system exhibits potential high-valued application of non-grain crops on producing HFS with D-allulose.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Shaochun Su,Li Hao,Huayao Chen,Xinhua Zhou,Hongjun Zhou
Sustainable food consumption is intertwined with sustainable agriculture development, which focuses on the production and protection of agricultural crops in a safe and effective fashion. Herein, amphiphilic functionalized chitosan oligosaccharide nanoparticles (CSD) were formed by a Schiff base reaction grafted with salicylaldehyde and D-(+)-galactose ( D -Gal). Avermectin (AVM) was used as a model pesticide and self-assembled onto CSD to obtain AVM@CSD nanoparticles with an encapsulation efficiency of 74.94%. AVM@CSD nanocarrier exhibited excellent anti-UV property to retain more AVM, due to their Schiff base structure and salicylaldehyde for UV shielding. Compared with bare AVM and commercial AVM emulsifiable concentrates, AVM@CSD preserved high insecticidal activity after UV irradiation . Additionally, CSD carrier promoted cucumber seed germination and seedling growth. These data suggested the potential utilization of the amphiphilic chitosan oligosaccharide as carriers for pesticides to improve their delivery and release properties and opens a novel avenue towards the application of water-dispersible and biological CSD in the field of pest management and plant growth.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xinlei Ji,Jia Kou,Gökalp Gözaydın,Xi Chen
Chitin biorefinery offers a unique opportunity to sustainably produce highly-valued organonitrogen compounds such as the versatile pharmaceutical precursor 3-acetamido-5-acetylfuran (3A5AF), bypassing the Haber process and mitigating the consumption of fossil feedstocks. However, the reported protocols engaged large quantities of toxic organic solvents and required harsh conditions. In this work, a highly efficient catalytic system has been developed in the nontoxic, biobased γ-valerolactone (GVL) solvent under relatively mild conditions. 3A5AF was selectively obtained with an unprecedent yield of 75.3% at 140 °C for 2 h by adding NH 4 SCN and HCl. The high yielding was exclusively promoted by a dissolution-dehydration effect. Based on the UPLC-TOF-MS and NMR analyses, the presence of NH 4 SCN has induced a very rapid NAG conversion possibly by coordinating with the acetamido group and the hydroxyl groups, and the 3A5AF product was obtained in a subsequent dehydration pathway from NAG with the Chromogen I and Chromogen III as the intermediates.
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Nano Research
·
2023
·Vol. 16
·期 8
·10748-10755
·
IF 9.9
Li Junhua,Jiang Yi,Zhang Xu,Huo Yidan,Du Fanglin,Tuo Yongxiao,Guo Zhiyan,Chen Dawei,Chen Shenghua
The electrooxidation of the alcohol and aldehyde molecules instead of water coupled with H 2 production has been proven to be effective for producing high-value fine chemicals under alkaline conditions. It is also noteworthy that under acidic conditions, the stability of non-noble metal water oxidation catalysts remains a great challenge due to the lattice oxygen mechanism. Hence, we coupled the biomass-derived glucose oxidation for high-value D-glucaric acid (GRA) with ultra-durable hydrogen in acid solution over a Yb-MnO 2 catalyst. The Mn 3+ regulated by Yb atoms doped in MnO 2 can effectively optimize the adsorption and desorption processes of the alcohol and aldehyde group and improve the intrinsic activity but cannot for H 2 O. The catalyst exhibited extremely high activity and stability after 50 h for glucose oxidation, inhibiting the lattice oxygen process and MnO 4− formation, while the activity was quickly lost within 0.5 h for water oxidation. Density functional theory (DFT) calculations further demonstrated that glucose oxidation reaction proceeds preferentially due to the oxidation of aldehyde group with lower adsorption-free energy (−0.4 eV) than water (Δ G > 0 eV), avoiding the lattice oxygen mechanism. This work suggests that biomass-derived glucose oxidation not only provides a cost-effective approach for high-value chemicals, but also shows an extremely potential as an alternative to acidic oxygen evolution reaction (OER) for ultradurable H 2 production.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Sundaram Chandrasekaran,Tingting Ma,Zhichang Hu,Qianying Liu,Chao Zhan,Yan Li,Chris Bowen,Huidan Lu,Yongping Liu
Chevrel-phase metal sulfides are known to be promising materials for energy conversion and storage applications. However, a detailed understanding of the intrinsic kinetic mechanisms of electrocatalytic bifunctional hydrogen and oxygen evolution reactions (HER/OER) on NiMo 3 S 4 -based Chevrel-phases is lacking. Herein, novel ultrathin self-assembled nanosheets of NiMo 3 S 4 are coupled with transition metal atoms (M/N-NiMo 3 S 4 ; where M = Co, Fe, and Cu) were formed by a facile hydrothermal approach. Notably, the Co/N-NiMo 3 S 4 electrocatalyst exhibits excellent performance in terms of ultralow overpotentials of 78, 208, 282, and 307 mV at 10, 100, 500, and 1000 mA cm −2 for the HER; and 186, 204, and 225 mV at 50, 100, and 300 mA cm −2 for the OER, respectively. Experimental and first principle calculations demonstrate that Co atoms coupling with edge Ni atoms results in d‐electron delocalization on Co/N-NiMo 3 S 4 , signifying the efficient charge transfer to improve overall water electrolysis. In addition, an upshift in the d‐band center of Co/N-NiMo 3 S 4 can optimize the free energies of a variety of reaction intermediates for water adsorption and dissociation; thereby facilitating the robust alkaline overall water electrolysis at 1.47 V. This work therefore greatly deepens the understanding of the bifunctional hydrogen and oxygen evolution reaction of Chevrel-phase electrocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xiaofei Liu,Tianxing Wang,Yilin Chen,Jingtao Wang,Wenjie Xie,Rongqian Wu,Xingtao Xu,Lihui Pang,Xiaogang Zhang,Yi Lv,Guangzhao Wang,Yusuke Yamauchi,Tian (Leo) Jin
Orbital hybridization is a powerful tool for modulating electronic structures toward various electrocatalytic reactions. Compared to the widely reported d - d hybridization in d -block metal alloys, the p - d orbital hybridization between d -block metals and p -block elements could provide new opportunities for regulating the electronic properties and thus promoting the electrocatalytic activities. Herein, we report a distinctive p -block metalloid-regulating p - d orbital hybridization to realize the fabrication of RuSb nanobranches for bifunctional hydrogen evolution (HER) and hydrazine oxidation (HzOR), which exhibits huge potential in overall hydrazine splitting (OHzS) by utilizing thermodynamically favorable HzOR instead of sluggish oxygen evolution on the anode. To our delight, RuSb delivers an impressively low overpotential of 39 mV for HER and 252 mV for HzOR at 10 mA cm −2 in alkaline seawater. The two-electrode OHzS electrolyzer with RuSb||RuSb couple can achieve outstanding electrocatalytic activity with an extraordinarily small cell voltage of 35 mV to drive 10 mA cm −2 in alkaline seawater, outperforming the Pt/C||Pt/C couple under the same condition. Density functional theory calculations further indicate that the Sb doping can not only mediate the adsorption energy for hydrogen but also the energy barrier for the dehydrogenation of *N 2 H 3 . Therefore, our work verifies the huge potential of p - d orbital hybridization for the development of a bifunctional OHzS system in alkaline seawater.
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INTERNATIONAL IMMUNOPHARMACOLOGY
·
2019
·
IF 3.361
Yutong He,Zijing Xia,Deqing Yu,Jiankang Wang,Liang Jin,Demin Huang,Xiaoli Ye,Xuegang Li,Baoshun Zhang
Acute liver failure (ALF) is a distinct clinical syndrome with high mortality and characterized by metabolic derangements, neurological complication , and multiple failures. Flavonoids exert great biological properties on anti-oxidation, anti-inflammation, and anti-apoptosis. After lipopolysaccharide (LPS)/ d -galactosamine ( d -GalN) administration, five flavonoids inhibited oxidative activities with reducing nitric oxide synthase (iNOS), malondialdehyde (MDA), and improving catalase (CAT), superoxide dismutase (SOD), total antioxidant capacity (T-AOC), nuclear factor erythroid-derived 2-related factor 2 (Nrf2) and heme oxygenase-1 (HO-1). They reduced the serum levels of alanine and aspartate aminotransferase (ALT, AST) and pro-inflammatory cytokines, prevented the phosphorylation of IKK, IκBα, and NF-κB/p65 in the NF-κB signaling pathway . Additionally five flavonoids inhibited hepatocyte apoptosis through increasing Bcl-2/Bax ratio and suppressing the Caspase family proteins. Chrysin , luteolin , apigenin , hesperetin and 3′, 4′-dimethoxy hesperetin have apparently hepato-protective effects against ALF induced by LPS/ d -GalN. The study found, the C2 C3 double bond at A ring, and the hydroxyl group of C3′ or C4′ at B ring increased the protective activities, however, the effect of hydroxymethylation at C3′ and C4′ was reversed. In addition, apigenin has good hepatoprotective effects and potential as a promising therapeutic agent for ALF in clinical application.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Xiaorong Zhang,Muhammad Shakeel,Baoshan Li,Muhammad Arif,Xianglong Kong,Jianjun Liu,Shengli Zuo
The present study is about the fabrication of an efficient photo-/electrocatalyst, prepared via in-situ hydrothermal coupling of ZnO with g-C 3 N 4 . The results prove this electrocatalyst as suitable band structure semiconductor. The crystalline nature and related morphological parameters are controlled by optimized hydrothermal and calcination temperatures conditions. A series of physicochemical characterization are applied to inquire the crystalline structure, surface morphology , optical capabilities and charge transportation properties. Results revealed that the sample acts as excellent electrocatalyst with OER current density at 10 mAcm −2 @ 335 mV and the HER at 100 mAcm −2 @ −225 mV. While upon illuminations its catalytic properties further enhance at OER 10 mAcm −2 @ 326 mV and for HER current density of 100 mAcm −2 @ −167 mV. It can be seen from the present study that g-C 3 N 4 play gigantic role in enhancing the catalytic property of ZnO and hence it leads to a relationship between hierarchical features and photo-/electrochemical activity for water splitting.
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ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Mengjie Wu,Hui Ma,Zhongyi Ma,Yufang Jin,Chunyan Chen,Xiaoya Guo,Yan Qiao,Christian Marcus Pedersen,Xianglin Hou,Yingxiong Wang
Deep eutectic solvents (DESs) exhibit similar physicochemical properties to the ionic liquids. They are inexpensive, renewable, nontoxic, and environmentally benign solvents and have gradually attracted attention in several fields, for example, biorefinery. Here choline chloride-based DESs have been used as solvents and catalysts for the preparation of deoxyfructosazine (DOF) through a self-condensation reaction of d-glucosamine (GlcNH2). The catalytic performances of a “green cocatalyst”, amino acids, and the reaction mechanism were also studied. The results displayed that choline chloride/urea was capable to convert GlcNH2 efficiently, with a 13.5% yield of DOF at low temperature and with a short reaction time (100 °C, 150 min). Among the screened amino acids, arginine showed the highest activity and gave the highest yield of DOF (30.1%) under the optimized reaction conditions. Nuclear magnetic resonance (NMR) studies revealed a strong hydrogen bond interaction between GlcNH2 and arginine. Moreover, a detectable intermediate, namely dihydrofructosazine, in the condensation of GlcNH2 to DOF/fructosazine (FZ) was captured by in situ NMR technique.
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TALANTA
·
2025
·
IF 6.1
Mingjiang Huang,Binbin Luo,Shengxi Wu,Miwan Shi,Yan Liu,Shenghui Shi
A D-Shaped, excessively tilted fiber grating (ExTFG) immunosensor modified with molybdenum disulfide (MoS 2 ) was developed for label-free and specific detection of growth-stimulated expressed gene 2 protein (ST2), a critical biomarker for heart failure. The D-Shaped ExTFG sensor was fabricated by side-polishing an ExTFG along its slow axis to enhance refractive index (RI) sensitivity. It was subsequently biofunctionalized with MoS 2 and anti-ST2 monoclonal antibodies (anti-ST2 MAbs) for ST2 immunoassays. The RI sensitivities of the sensor after side-polishing and MoS 2 coating were thoroughly investigated. Additionally, the immunodetection properties of the sensor were evaluated across varying concentrations of ST2 antigen solutions, as well as its specificity and clinical performance in serum samples from healthy individuals and patients. Experimental results revealed that the sensitivity of the MoS 2 -modified D-Shaped ExTFG immunosensor for ST2 reached 0.335 nm/[log(mg/mL)] over a wide linear testing range of 1 ng/mL to 1000 ng/mL, with a detection limit of 0.472 ng/mL. This represents an improvement of approximately 86 % compared to the ExTFG without D-Shaped modification and demonstrates excellent specificity for ST2 biomarkers even in complex clinical sera. The MoS 2 -modified D-Shaped ExTFG immunosensor exhibits notable advantages, including stability, practical usability, and high clinical specificity, making it a promising candidate for biomedical and other analytical applications.
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