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Molecular Catalysis · 2019 · IF 2.938

Simple synthesis of WO3-Au composite and their improved photothermal synergistic catalytic performance for cyclohexane oxidation

Jijin Mai,Yanxiong Fang,Jincheng Liu,Jinhong Zhang,Xiaolan Cai,Yuying Zheng

Partial oxidation of cyclohexane (CHA) to KA oil (cyclohexanone (-one) and cyclohexanol (-ol)) with dry air is one of the most important industrial process. Despite great efforts have made in developing new catalysts, industrial processes are still limited by low conversion and selectivity with harsh condition. Here we report a significantly improved cyclohexane conversion and KA oil selectivity under solar light irradiation by anew photothermal synergistic catalyst, which was prepared by loading Au nanoparticles (Au NPs) onto WO 3 nanosheets (WO 3 NSs) with simple ultrasonic method. A high conversion of 9.0% and a high selectivity of 99.0% are acquired by WO 3 nanosheets-Au nanoparticles (WO 3 -Au) composite under dry air, which are much higher than the simple sum of photocatalysis and thermal catalysis. The significantly improved catalytic properties of cyclohexane oxidation by the WO 3 -Au composite are mainly attributed to the improved light absorption, the effective charge separation and the synergistic effect of photocatalysis and thermal catalysis. The photothermal synergy to improve catalytic activity may be widely used in green industrial catalytic processes.

研究领域: 催化化学 · 材料科学 · 环境科学
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ACS Nano · 2020 · IF 14.588

Protein Binding Affinity of Polymeric Nanoparticles as a Direct Indicator of Their Pharmacokinetics

Zhi-Ting Cao,Li-Qin Gan,Wei Jiang,Ji-Long Wang,Hou-Bing Zhang,Yue Zhang,Yucai Wang,Xianzhu Yang,Menghua Xiong,Jun Wang

Polymeric nanoparticles (NPs) are an important category of drug delivery systems, and their in vivo fate is closely associated with delivery efficacy. Analysis of the protein corona on the surface of NPs to understand the in vivo fate of different NPs has been shown to be reliable but complicated and time-consuming. In this work, we establish a simple approach for predicting the in vivo fate of polymeric NPs. We prepared a series of poly(ethylene glycol)-block-poly(d,l-lactide) (PEG-b-PLA) NPs with different protein binding behaviors by adjusting their PEG densities, which were determined by analyzing the serum protein adsorption. We further determined the protein binding affinity, denoted as the equilibrium association constant (KA), to correlate with in vivo fate of NPs. The in vivo fate, including blood clearance and Kupffer cell uptake, was studied, and the maximum concentration (Cmax), the area under the plasma concentration–time curve (AUC), and the mean residence time (MRT) were negatively linearly dependent, while Kupffer cell uptake was positively linearly dependent on KA. Subsequently, we verified the reliability of the approach for in vivo fate prediction using poly(methoxyethyl ethylene phosphate)-block-poly(d,l-lactide) (PEEP-b-PLA) and poly(vinylpyrrolidone)-block-poly(d,l-lactide) (PVP-b-PLA) NPs, and the linear relationship between the KA value and their PK parameters further suggests that the protein binding affinity of polymeric NPs can be a direct indicator of their pharmacokinetics.

CAS / MDL: 34215-57-1
研究领域: 纳米技术 · 药剂学 · 生物材料科学
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JOURNAL OF CATALYSIS · 2023 · IF 7.3

Evidence of C–H bond activation dominating in both C6H12 oxidation and consequential C–C bond rupture

Jin Yuan,Zhiwei He,Hongbo Zhang

Selective C–H bond oxidation of cyclohexane into KA oil (ketone-alcohol) is of vital importance in both fundamental research and industrial applications while limited by complex reaction network and suffering from low efficiency. In this study, Ce(OH)SO 4 · x H 2 O was chosen as a probe to systematically investigate the C–H bond activation and C–C bond rupture as a function of various reaction parameters, including the reactant/product concentrations, catalyst applied, reaction temperatures, acidic concentrations etc, and found that bi-molecule of C 6 H 12 was probably involved in both C–H bond rupture and C–C bond cleavage and both were controlled by one deprotonation elementary step with ·O 2 – and h + as the key active components, which were supported by parity fittings and primary KIEs determined. In addition, the C–C bond rupture was found to be mainly following C 6 H 10 O to ε-caprolactone and further to linear acids reaction path. Hopefully, this study could help people find/optimize reaction systems in selective hydrocarbon upgradings.

研究领域: 化学工程 · 有机化学 · 催化
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-16 · IF 14.7

Electrosynthesis of adipic acid with high faradaic efficiency within a wide potential window

Liu Xiang,Zhu Yu-Quan,Li Jing,Wang Ye,Shi Qiujin,Li An-Zhen,Ji Kaiyue,Wang Xi,Zhao Xikang,Zheng Jinyu,Duan Haohong

Electrosynthesis of adipic acid (a precursor for nylon-66) from KA oil (a mixture of cyclohexanone and cyclohexanol) represents a sustainable strategy to replace conventional method that requires harsh conditions. However, its industrial possibility is greatly restricted by the low current density and competitive oxygen evolution reaction. Herein, we modify nickel layered double hydroxide with vanadium to promote current density and maintain high faradaic efficiency (>80%) within a wide potential window (1.5 ~ 1.9 V vs. reversible hydrogen electrode). Experimental and theoretical studies reveal two key roles of V modification, including accelerating catalyst reconstruction and strengthening cyclohexanone adsorption. As a proof-of-the-concept, we construct a membrane electrode assembly, producing adipic acid with high faradaic efficiency (82%) and productivity (1536 μmol cm −2 h −1 ) at industrially relevant current density (300 mA cm −2 ), while achieving >50 hours stability. This work demonstrates an efficient catalyst for adipic acid electrosynthesis with high productivity that shows industrial potential.

研究领域: 化学工程 · 电化学 · 材料科学 · 可持续化学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Development of bovine serum albumin-modified Fe3O4 embedded in porous α-ketoglutaric acid/chitosan (BSA/Fe3O4@KA/CS): A magnetically targeted hemostatic dressing for deep and irregular wounds

Jinnan Guo,Yuanyuan Zhao,Guanqun Peng,Tong Ye,Xiaohui Zhu,Runtian Li,Jintao Shen,Lina Du,Shanshan Wang,Zhiyun Meng,Hui Gan,Ruolan Gu,Wenzhong Sun,Guifang Dou,Shuchen Liu,Yunbo Sun

Severe bleeding from deep and irregular wounds poses a significant challenge in prehospital and surgical settings. To address this issue, we developed a novel chitosan-based hemostatic dressing with a magnetic targeting mechanism using Fe 3 O 4 , termed bovine serum albumin-modified Fe 3 O 4 embedded in porous α-ketoglutaric acid/chitosan (BSA/Fe 3 O 4 @KA/CS). This dressing enhances hemostasis by magnetically guiding the agent to the wound site. In vitro, the hemostatic efficacy of BSA/Fe 3 O 4 @KA/CS is comparable to that of commercial chitosan (Celox™) and is not diminished by the modification. In vivo, BSA/Fe 3 O 4 @KA/CS demonstrated superior hemostatic performance and reduced blood loss compared to Celox™. The hemostatic mechanism of BSA/Fe 3 O 4 @KA/CS includes the concentration of solid blood components through water absorption, adherence to blood cells, and activation of the endogenous coagulation pathway. Magnetic field targeting is crucial in directing the dressing to deep hemorrhagic sites. Additionally, safety assessments have confirmed the biocompatibility and biodegradability of BSA/Fe 3 O 4 @KA/CS. In conclusion, we introduce a novel approach to modify chitosan using magnetic guidance for effective hemostasis, positioning BSA/Fe 3 O 4 @KA/CS as a promising candidate for managing various wounds.

研究领域: 生物材料 · 止血 · 伤口愈合 · 纳米技术 · 生物医学工程
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TALANTA · 2023 · IF 6.1

A novel fluorescent probe for the detection of peroxynitrite and its application in mice epileptic brain model

Guanyi Lu,Haowen Fan,Kaidong Wang,Gaonan Tian,Chaoyan Chen,Yao Wang,Lei Wang,Xiangjun Fan

Herein, a fluorescent probe, GYP , was developed for the detection of ONOO − in KA-induced epileptic brains. In solution, as a ratiometric probe, GYP indicated practical properties including steadiness under wide pH range (3.0–12.0), rapid response (within 20 s), stability over 48 h, high sensitivity (LOD = 0.27 μM) and high selectivity. In living PC12 cells, in spite of the low toxicity, GYP could achieve the time-dependent and dose-dependent imaging of ONOO − , while the generation and elimination were checked by introduction of SIN-1 and NAC, respectively. Further, GYP could cross Blood-Brain Barrier (BBB) rapidly and steadily during the imaging in KA-induced mice epileptic brain model. Thus, this work raised a practical implement for the detection of ONOO − in brain region, which might be helpful for further understanding of the epilepsy mechanism in future.

研究领域: 神经科学 · 化学 · 药理学
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