JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Shuchun Li,Xuefei Zhang,Xiaoyan Huang,Shuchang Wu,Zailai Xie
Developing highly active and stable nanocarbon catalysts for selective oxidation reactions has attracted much attention due to their potential as an alternative to traditional metal-based or noble metal catalysts. However, the nature of active sites and the reaction mechanism of nanocarbon catalysts for oxidation reactions still remains largely unknown, which hinders the rational design and development of highly efficient carbon-based catalysts. Here we report a facile strategy for the synthesis of boron and nitrogen co-doped carbon nanosheet material (BNC), which exhibits excellent catalytic activity with 91% conversion and 99% selectivity in selective oxidation of benzyl alcohol into benzaldehyde, superior to those of traditional carbon materials (oxidized carbon nanotubes, graphites and commercial nanocarbons). Structural characterizations and kinetic measurements are studied to clarify the active site, in which phenolic hydroxyl on BNC is responsible for the production of benzaldehyde. Meanwhile, we put forward a possible reaction mechanism and point out the key factors in determining the reactivity for this reaction. Therefore, the present work provides new insight into structure–function relationships, paving the way for the development of highly efficient nanocarbon catalysts.
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Science China-Chemistry
·
2022
·Vol. 65
·期 8
·1661-1669
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IF 10.138
Pu Chun,Li Rui-Dong,Chang Gang-Gang,Chen Min-Jie,Yao Yao,Li Jun-Sheng,Zhao Bo,Wu Lu,Zhang Yue-Xing,Yang Xiao-Yu
Carbon supported metal catalysts have received considerable interest due to their widespread applications in heterogeneous catalysis. However, the controllable synthesis of carbon support with defined morphology and composition still represents great challenging. Herein, we reported the synthesis of a well-defined hierarchically nanosized H-ZrO 2 /NC (nitrogen-doped carbon) network via an inheritable carbonization strategy. When immobilizing the palladium clusters into the support, the N-doped sites and oxygen vacancy of the carbon composite can effectively stabilize and activate Pd through strong metal-support interaction which was also confirmed by density functional theory (DFT) calculations. Moreover, the hierarchically nanosized network can contribute to the exposure of active sites and facilitate the mass transfer during the catalytic process. As a result, benefiting from the hierarchical structure, composition and hydrolytic nature, Pd@H-ZrO 2 /NC exhibited excellent catalytic activity and stability towards the hydrogenation of furfural in mild reaction conditions, as well as good universality toward the hydrogenation of a series of unsaturated hydrocarbons.
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EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
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2018
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IF 4.816
Kun Chen,Ya-Liang Zhang,Jing Fan,Xiang Ma,Ya-Juan Qin,Hai-Liang Zhu
In the present work, twenty-five nicotinoyl pyrazoline derivates bearing N-methyl indole moiety have been designed and synthesized. The biological evaluation of these compounds as tubulin assembly inhibitors revealed that most of them were potential antitumor agents . Among them, compound 28 exhibited most potency against cancer cell line panels (GI 50 = 29–90 nM for HeLa, HepG2 and MCF-7 cells) without toxicity to non-tumor cells (CC 50 > 300 μM for 293 T cell), bound to the colchicine site of tubulin and displayed excellent inhibitory activity in tubulin assembly assay (IC 50 = 1.6 μM, better than CA-4). Molecular dynamics simulation was carried out to validate the docking pose of compound 28 with tubulin crystalline. Further investigation on HepG2 and HeLa cells demonstrated that compound 28 could cause mitosis arrest to G2/M phase, and subsequently induced cell apoptosis . The efficiency in vivo of compound 28 was also evaluated on HeLa-Xenograft nude mice , and the relative tumor inhibition ration was up to 61.52% without noticeable weight loss and tissue damage (examined by H&E staining), which was comparable to CA-4 (inhibited 59.92%). In brief, compound 28 is a promising candidate for tumor therapy as tubulin assembly inhibitor.
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Nano Energy
·
2026
·
IF 16.7
Nan Shi,Jianyao Xu,Xiaofang Shi,Yarong Lan,Peiyi Wu,Zhiguo Hu
Novel anti-swelling ionic liquid hydrogel was prepared via a pioneering one-pot hydrophobic crosslinked strategy. • The material strikes a synergistic balance among mechanical toughness, ionic conductivity, freeze resistance and thermoelectric performance. • The high thermoelectric Property and the internal selective regulation mechanism was systematically revealed. Ionic thermoelectric cells (i-TECs) can convert low-grade heat into electricity, but achieving stable performance across wide temperatures range with high thermopower and good mechanical durability remains difficult. This study presents a hydrophobic crosslinking strategy to fabricate fatigue-resistant hydrogel P(NAGA-co-VEIMBr) (PNVC) in one step. The hydrophobic macromolecular crosslinker imparts strong anti-swelling for importing thermoelectric ions. PNVC-based i-TECs show high thermoelectric performance, reversible elasticity, and excellent freeze resistance, allowing stable operation from −20 to 60 °C. The optimized PNVC i-TEC device achieves a thermopower of −10.86 mV K⁻¹ above 0 °C and −4.52 mV K⁻¹ subzero, along with a Young’s modulus of 0.21 MPa. A six-unit array can power an LED by harvesting body heat. PNVC i-TECs also enable self-powered multimodal sensing through small changes in resistance, voltage, or current, demonstrating its exceptional capability for self-powered sensing integrated applications. This hydrophobic crosslinking strategy offers a promising solution for facilely fabricate high performance ionic i-TE materials. Download: Download high-res image (164KB) Download: Download full-size image Table of contents entry An anti-fatigue, freeze-resistant hydrogel ionic thermoelectric cell is fabricated using a hydrophobic crosslinking strategy. It shows high thermoelectric performance, reversible elasticity, and excellent self-healing performance, allowing stable operation over a wide temperature range. These features make it a top-performing i-TEC. The simple fabrication method provides valuable insights for developing high-performance, multifunctional thermoelectric cells.
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PROGRESS IN ORGANIC COATINGS
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2023
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IF 6.6
Yufa Sun,Hao Xin,Yi Wu,Chen Zhang,Changjie Chen,Xiangdong Zhou
A new type of flame-retardant polyether diols containing phosphorus, nitrogen, and sulfur (SPAE) was first synthesized by using phosphoryl chloride, 2-aminobenzothiazole and ethylene glycol . The SPAE as the soft segment was then utilized to prepare a series of flame-retardant waterborne polyurethanes (SPAE-WPU) through emulsion polymerization . Subsequently, SFR-WPU as a finishing agent was coated on polyamide fabric. When the content of SPAE-WPU was 18 wt%, the coated fabric exhibited a limiting oxygen index (LOI) of 28.2 %, afterflame time of 4.6 s, afterglow time of 0 s and damaged length of 11.2 cm, respectively. After 10 washes, the coated fabric retained its good flame-retardancy and anti-dripping properties. Furthermore, the flame-retardant mechanism of SPAE-WPU was investigated using various spectral analyses, which revealed that the P, N and S elements worked together to create non-combustible gas compounds, release free radicals, and promote dehydration and carbonization , leading to synergistic flame-retardant effects in both gas- and condensed-phase.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Xiaoyan Xu,Qihong Lu,Jiawei Wu,Wei Mo,Lei Zuo,Ning Yang,Weiwei Xia,Xianghua Zeng
To improve CdS photocatalytic activity , both Cu x Cd 1- x S nanorods and Cu 2 S@CdS p-n heterostructures have been prepared with a simple solvothermal method . The results showed that the maximum H 2 generation rate is equal to 10 mmol h −1 g −1 and 12.1 mmol h −1 g −1 for samples 0.3-Cu 2 S@CdS and Cu 0.1 Cd 0.9 S, respectively, which are nearly 9 and 12 times larger than that of CdS (1.2 mmol h −1 g −1 ) without using Pt as the co-catalyst. The measurements of the light absorption revealed that the samples Cu 2 S@CdS p-n heterostructures and Cu x Cd 1- x S nanorods have an increased visible light absorption. Band structure revealed that Cu 2 S@CdS p-n composite is a type-II heterostructure, which facilitates the separation of photoexcited charge carriers . Furthermore, as the Cu-doping CdS introduced a defect level , which induced the increase of carrier density, and the defect energy level in Cu 0.1 Cd 0.9 S and the band energy in CdS form a type-II heterostructure. Due to the appropriate band structure and stronger light absorption, Cu 2 S@CdS p-n heterostructures and Cu + -doping CdS demonstrated an improved photocatalytic activity and stability.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Jianwang He,Zhijin Cheng,Zhuo Liu,Meijuan Yin,Yuchi Zhang,Le Han,Yan Xu
Although metal oxides based gas sensors have been researched extensively in previous works, there are enormous challenges on improving the deficiencies in poor selectivity, sensitivity, humidity resistance and so on. Hence, we developed an epitaxial growth method to prepare dendritic Co 3 O 4 /In 2 O 3 -(1−3) heterostructures of distinct Co/In mass ratios through perfect lattice matching between the two crystal domains at the interface, along with introducing large amounts of oxygen vacancies . As a result, the Co 3 O 4 /In 2 O 3 -2 heterostructure based gas sensor showed enhanced sensing properties towards triethylamine (TEA, 100 ppm) with a high response value of Ra/Rg = 576.1 at an optimal working temperature of 200 °C, which is 93 times higher than that of pristine In 2 O 3 . Moreover, the Co 3 O 4 /In 2 O 3 -2 sensor exhibited excellent gas selectivity, quick recovery time, repeatable cycling, long-term stability, as well as outstanding humidity resistance. The improved TEA gas sensing performance can be attributed to the integration of interfacial synergies in Co 3 O 4 /In 2 O 3 p-n heterostructure and generation of rich oxygen vacancies, exposing more active sites to facilitate the adsorption/desorption of gas molecules. This work provides a feasible pathway to regulate TEA sensing performance of metal oxide semiconductor (MOS) gas sensors by capitalizing on self-sacrificial template strategy and reconstruction of novel metal oxide heterostructure.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Haiqiang Mu,Yu-An Li,Xiuli Wang,Feng Li,Xin Du,Jing Li
The rational modulation of the coordination environment of the active center of single-atom catalysts (SACs) is a potential strategy to improve the activity and selectivity of electrocatalytic CO 2 reduction. We developed a series of single-atom Ag-anchored on N -doped carbon catalysts with different N -coordination environments by regulating the carbon source (glucose/graphene oxide, GO). Results demonstrated that the CO 2 -to-CO/C 2 H 5 OH pathway can be converted through reasonable regulation of the content of pyrrolic N and pyridine N. At a highly dominant pyrrolic N content of 40.0 %, the electrocatalyst of Ag-N-rGO 0.025 M facilitates the formation of CO with a Faradaic efficiency (FE) of 69.7 %. By contrast, when the pyridine N content is 70.5 %, the best Ag-N-C 0.05 M catalyst in the H-cell shows an FE of 42 % for C 2 H 5 OH at −0.97 V vs. RHE; moreover, the FE is stable at 40 % within 31 h. Density functional theory calculations further confirm that the pyrrolic N site is conducive to the conversion of CO 2 to intermediate *CO, whereas pyridine N exhibits the highest binding energy (ΔG = -4.73 eV) to hold *CO intermediates for dimerization, consequently steering the pathway to the formation of C 2 H 5 OH. The results of this study provide novel insights into the rational design of carbon-based SACs based on efficient electrochemical CO 2 reduction reaction and the regulation of CO 2 selectivity and activity for C 2 H 5 OH production.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Yuyang Liu,Qiong He,Yarong Li,Yongqiang Li,Chiyang He
The main challenge of using non-noble metal copper nanoparticles (Cu NPs) as catalysts is to find or prepare suitable support platforms to anchor Cu NPs, thereby avoiding the aggregation tendency owing to their high surface energy. In this study, a novel pyridine N-containing covalent organic framework (COF) was designed and used as a template for the confined growth of Cu NPs. The prepared imine-connected TAPB-PCBA had abundant one-dimensional ordered channels, moderate specific surface area and good stability. The skeleton structure of TAPB-PCBA contained a large number of evenly distributed pyridine N, which can act as the nucleation site for Cu NPs. The well-defined pore structure confines the growth of Cu NPs and makes them controllable in size. The pores in TAPB-PCBA are completely independent and isolated from each other, minimizing the accumulation of Cu NPs. With the help of these factors, ultrafine Cu/Cu 2 O composite NPs (2.5 nm) with narrow size distribution anchored inside the cavity of the TAPB-PCBA were successfully prepared. The as-prepared Cu-containing COF, Cu@TAPB-PCBA, showed excellent catalytic capacity for dye degradation and nitrophenol reduction under mild conditions and low catalyst loads, respectively. In addition, Cu@TAPB-PCBA also has a good recyclability, multiple use without significant loss of catalytic activity. We expect this COF-supported growth-confined preparation of metal NPs to further facilitate the design and preparation of non-noble metal NPs@ COF composites, replacing noble metals in certain catalytic applications.
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Water
·
2023
·Vol. 15
·期 20
·3670
·
IF 3.4
Xiaosong Zha,Shuren Wang,Deyu Zhang
N-nitrosodimethylamine (NDMA), as an emerging nitrogenous disinfection byproduct, is strictly controlled by multiple countries due to its high toxicity in drinking water. Advanced reduction processes (ARPs) are a new type of water treatment technology that can generate highly reactive reducing radicals and make environmental contaminants degrade rapidly and innocuously. In this study, a systematic investigation on the kinetics of the NDMA degradation via the chosen UV/sulfite ARP and the impacts of some key parameters of reaction system was conducted. The results indicated that the UV/sulfite ARP was an efficient and energy saving method for the reductive degradation of NDMA. A total of 94.40% of NDMA was removed using the UV/sulfite ARP, while only 45.48% of NDMA was removed via direct UV photolysis under the same reaction conditions. The degradation of NDMA via the UV/sulfite ARP followed pseudo-first-order kinetics. Increasing both the UV light intensity and sulfite dosage led to a proportional increase in the NDMA removal efficiency. The alkaline condition favored the degradation of NDMA, with the removal efficiency increasing from 21.57% to 66.79% within the initial 5 min of the reaction when the pH increased from 3 to 11. The presence of dissolved oxygen substantially decreased the removal efficiency of NDMA due to the formation of oxidizing superoxide radicals, which competed with NDMA by capturing the reducing active radicals during the reaction. An analysis of the degradation products indicated that several refractory intermediates such as dimethylamine, methylamine and nitrite were completely decomposed via the UV/sulfite ARP, and the final degradation products were formate, ammonia and nitrogen.Keywords:N-nitrosodimethylamine;UV/sulfite ARP;reductive degradation;influencing factors;mechanism
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 45
·21024-21032
·
IF 3.3
Weilin Shen,Dawson Wai-Shun Suen,Eric Tung-Po Sze,Xiao Chen,Changhai Liang,Chi-Wing Tsang
The water splitting reaction has the potential to be a sustainable and environmentally friendly way of producing hydrogen as a fuel source, which is an important step in reducing our reliance on fossil fuels and mitigating climate change. Currently, most commonly used catalysts for water splitting are based on precious metals such as platinum and iridium, which are expensive and scarce. Therefore, finding new catalysts that are low-cost, abundant and efficient is of great importance for making water splitting economically viable on a large scale. It was found that pairing up Co nanoparticles (NPs) with MoCx boosted the hydrogen evolution reaction (HER) activity by more than 2-fold (η10 = 130 mV, Tafel slope = 156.08 mV dec−1), compared with the pure Co NPs supported on N-doped carbon (η10 = 337 mV) under alkaline medium conditions. Its activity is comparable to those of Pt single-atom catalysts (SACs) supported on a mesoporous carbon matrix. The good activity may be due to the modification of the D-band of Co by Mo doping and the relatively high electrochemically active surface area (ECSA) of 477.25 cm2, which is comparable to those of Ru SAC materials.
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Polymers
·
2023
·Vol. 15
·期 21
·4335
·
IF 5
Zhuo Chen,Qinghua Zhao,Jiahui Chen,Tao Mei,Wenwen Wang,Mufang Li,Dong Wang
Polypropylene melt-blown nonwoven fabric (PP MNF) masks can effectively block pathogens in the environment from entering the human body. However, the adhesion of surviving pathogens to masks poses a risk of human infection. Thus, embedding safe and efficient antibacterial materials is the key to solving pathogen infection. In this study, stable chlorinated poly(methacrylamide-N,N′-methylenebisacrylamide) polypropylene melt-blown nonwoven fabrics (PP-P(MAA-MBAA)-Cl MNFs) have been fabricated by a simple UV cross-link and chlorination process, and the active chlorine content can reach 3500 ppm. The PP-P(MAA-MBAA)-Cl MNFs show excellent hydrophilic and antibacterial properties. The PP-P(MAA-MBAA)-Cl MNFs could kill all bacteria (bothEscherichia coliandStaphylococcus aureus) with only 5 min of contact. Therefore, incorporating PP-P(MAA-MBAA)-Cl MNF as a hydrophilic antimicrobial layer into a four-layer PP-based mask holds great potential for enhancing protection and comfort.Keywords:polypropylene melt-blown nonwoven fabric;antibacterial materials;UV irradiation;superhydrophilicity;N-halamine
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