DIAMOND AND RELATED MATERIALS
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2023
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IF 4.1
Yuhao Han,Jin Lin,Huajun Zhou,Li Guo,Yanzhong Wang
Developing an efficient non-noble metal catalyst for water splitting is very important for large-scale production of green hydrogen , but it is still a challenge due to the slow kinetics of hydrogen evolution in alkaline media . Herein, the self-standing Co 2 P 2 O 7 encapsulated N doped carbon anchoring onto the skeletons of carbon foams (Co 2 P 2 O 7 @NC/CF) was synthesized via the phosphating and carbonization of zeolitic imidazolate framework cross-shaped nanosheets at different temperatures. Co 2 P 2 O 7 @NC/CF-700 showed the highest HER activity, with an overpotential of 145.7 mV and a Tafel slope of 92.6 mV dec −1 at a current density of 10 mA cm −2 . Such an excellent performance is attributed to the three-dimensional interconnected, conductive carbon foams (CF) and uniformly distributed cross-shaped Co 2 P 2 O 7 @NC nanosheets, resulting in exposing more active sites and facilitating the mass and electron transfer .
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Yanzhong Wang,Sha Li,You Chen,Xiaofeng Shi,Chao Wang,Li Guo
Developing efficient Pt-free electrochemical catalysts for hydrogen evolution reaction (HER) is crucial for an energy source with low pollutant emissions. Herein, zeolitic imidazolate framework-67 (ZIF-67) polyhedrons are first in situ grown on the fibrils of commercial melamine foam at room temperature, and then phosphided and carbonized to obtain the free-standing 3D hierarchical CoP@N-doped carbon composite foam (CoP@NC/CF) with interconnected architecture. The 3D interconnected carbon networks provide efficient and fast channels for the rapid transfer of ions and electrons, and inhibit the agglomeration of CoP nanoparticles . The unique structure of CoP@NC/CF thus allows for delivering the remarkable HER performance with a low overpotential of 151.3 mV at 10 mA cm −2 , small Tafel slope of 64.8 mV dec −1 , and excellent long-term stability. This research provides a new strategy for the rational design and facile synthesis of the free-standing 3D CoP-based catalysts for high-performance HER.
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JOURNAL OF MEDICINAL CHEMISTRY
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2014
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IF 5.48
Yuanchao Xie,Dongqing Xu,Bing Huang,Xiuli Ma,Wenbao Qi,Fangyuan Shi,Xinyong Liu,Yingjie Zhang,Wenfang Xu
To discover group-1-specific neuraminidase (NA) inhibitors that are especially involved in combating the H5N1 virus, two series of oseltamivir derivatives were designed and synthesized by targeting the 150-cavity. Among these, compound 20l was the most potent N1-selective inhibitor, with IC50 values of 0.0019, 0.0038, and 0.0067 μM against NAs from three H5N1 viruses. These values are better than those of oseltamivir carboxylate. Compound 32 was another potent N1-selective inhibitor that exhibited a 12-fold increase in activity against the H274Y mutant relative to oseltamivir carboxylate. Molecular docking studies revealed that the 150-cavity was an auxiliary binding site that may contribute to the high selectivity of these compounds. The present work is a significant breakthrough in the discovery of potent group-1-specific neuraminidase inhibitors, which may be further investigated for the treatment of infection by the H5N1 virus.
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PubMed
高影响因子
Materials Horizons
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2023
·Vol. 11
·期 4
·1023-1031
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IF 13.3
Weichen Song,Jiankun Sun,Qian Wang,Han Wu,Kunpeng Zheng,Binbin Wang,Zhong Wang,Xiaojing Long
Organic semiconductor (OSC) gas sensors with good mechanical flexibility have received considerable attention as commercial and wearable devices. However, due to poor resistance to moisture and low conductivity, the improvement in the sensing capability of individual OSCs is limited. Reported here is a promising pathway to construct a series of conjugated organic polymers (COPs) with well-defined pyrimidine (Py-COP) or boron β-diketone (BF-COP) units. Unlike traditional metal- or carbon-based hybrid materials, the developed COPs can provide abundant absorption sites for gaseous analytes. As a result, the as-prepared BF-COP results in an excellent sensing response of over 1500 (Ra/Rg) toward 40 ppm of NH3 at room temperature, which is the highest value among those of pristine COPs as n-type sensing materials. Notably, they can maintain their initial sensing responses for two months and 90% relative humidity resistance. Combining the results of in situ Fourier transform infrared spectroscopy and theoretical calculations, the β-diketone skeleton is found to activate the surface electronic environment, verifying that the electron-deficient B ← O groups are adsorption centers. The B/N-heterocyclic decoration effectively modulates the redox properties and electronic interactions, as well as perturbs charge transfer in typical π-conjugated COPs. These results offer insight into developing highly efficient OSC gas sensors, which potentially have broadened sensing applications in the areas of organoboron chemistry.
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APPLIED CATALYSIS A-GENERAL
·
2026
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IF 4.8
Yu Han,Yu-Wei Xiang,Zhi-Rong Fu,Xin Zhang,Jia-Yi Zhou,Xiang-Sen Wu,Yong Luo
The 8H-NEC was synthesized by different organic routes and used as the substrate for kinetic studies. • Ru/Al 2 O 3 catalysts with controllable Ru particle sizes were prepared. • Smaller Ru particles showed higher TOF and lower apparent activation energy. • Low-coordinated Ru line-edge sites enhanced 8H-NEC adsorption. N -ethylcarbazole (NEC) is a promising liquid organic hydrogen carrier (LOHC) for hydrogen storage, and Ru/Al 2 O 3 catalyst is one of the most widely used catalysts for NEC hydrogenation. However, previous studies have primarily focused on the chemical electronic effect of Ru/Al 2 O 3 catalyst, while neglecting the influence of geometric structure. In this work, Ru particle size effect on the rate-determining step of 8H- N -ethylcarbazole (8H-NEC) hydrogenation has been considered. Firstly, a series of Ru/Al 2 O 3 catalysts with controllable Ru particle sizes were prepared. After that, 8H-NEC was synthesized by different organic routes to serve as the substrate for catalytic and kinetic experiments. Results showed that as the Ru particle size increased from 1.4 to 5.3 nm, the turnover frequency (TOF) decreased from 59.7 to 32.2 min −1 and the apparent activation energy increased from 44.55 to 74.00 kJ·mol −1 . CO probe diffuse reflection infrared Fourier transform spectrum (CO-DRIFTS) and density functional theory (DFT) results demonstrated that superior catalytic performance of smaller Ru particles was associated with the exposure of more low-coordinated line-edge sites, which exhibited stronger adsorption toward 8H-NEC. This study offers new insights into the design of highly efficient catalysts of NEC hydrogenation. Download: Download high-res image (169KB) Download: Download full-size image
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JOURNAL OF CHROMATOGRAPHY B-ANALYTICAL TECHNOLOGIES IN THE BIOMEDICAL AND LIFE SCIENCES
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2023
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IF 3
Haiyan Chen,Xinyu Wang,Meijin Lv,Yongxin She,Ziping Zhang,Xiaolin Cao
In this paper, the novel metal-organic framework @molecularly imprinted polymers were prepared and applied in extracting N-nitrosamines from salted vegetables. The imprinted polymers were coated on the surface of MIL-101 using multi-dummy template molecules (5-nonanol, benzhydrol and N-formylpyrrolidine). The characterization and adsorbing experiments showed that the hybrid imprinted polymers presented spherical particles with typically core-shell structure, and exhibited high adsorption capacity (maximum capacity: 46.85 mg/g) and fast equilibrium rate (only 5 min) for N-nitrosamines. Various parameters (sample loading solvent, pH, washing solvent, elution solvent and elution volume) affecting solid-phase extraction were optimized. Under the optimum conditions, the solid-phase extraction process based on the hybrid polymers combined with high performance liquid chromatography-ultraviolet detection method was established and applied to analyze N-nitrosamines in different salted vegetables. The results showed that the developed method produced the linear relationship between the peak areas versus the N-nitrosamines concentrations of 0.2–10 µg/g with limit of detections from 20.6 to 76.1 ng/g. The spiked recovery of N-nitrosamines in the salted vegetable samples was in the range of 66–100.5 % with relative standard deviation from 0.1 to 3.4 %. Those results demonstrated that the established method was sensitive and efficient for directly enriching and analyzing trace N-nitrosamines in salted vegetables.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Yonghai Feng,Min Yu,Minjia Meng,Lei Liu,Dewei Rao
In the selective oxidation of biomass-based 1,2-propanediol (PDO) with oxygen as the terminal oxidant, it is challenging to improve the lactic acid (LA) selectivity for nonnoble metal nanoparticles (NPs) due to their limited oxygen reduction rate and easy C–C cleavage. Given the high economic feasibility of nonnoble metals, i.e., Cu, in this work, copper and nitrogen codoped porous carbon nanosheets encapsulating ultrafine Cu nanoparticles (Cu@Cu-N-C) were developed to realize highly selective of PDO oxidation to LA. The carbon-encapsulated ultrasmall Cu 0 NPs in Cu@Cu-N-C have high PDO dehydrogenation activity while N-coordinated Cu (Cu-N) sites are responsible for the high oxygen reduction efficacy. Therefore, the performance of catalytic PDO conversion to LA is optimized by a proposed pathway of PDO → hydroxylacetone → lactaldehyde → LA. Specifically, the enhanced LA selectivity is 88.5%, and the PDO conversion is up to 75.1% in an O 2 -pressurized reaction system (1.0 MPa O 2 ), superior to other Cu-based catalysts, while in a milder nonpressurized system (O 2 flow rate of 100 mL min −1 ), a remarkable LA selectivity (94.2%) is obtained with 39.8% PDO conversion, 2.2 times higher than that of supported Au nanoparticles (1% Au/C). Moreover, carbon encapsulation offers Cu@Cu-N-C with strong leaching resistance for better recycling.
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INTERNATIONAL JOURNAL OF REFRACTORY METALS & HARD MATERIALS
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2023
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IF 3.6
Mengxian Zhang,Xianrui Zhao,Junting Zhang,Zhigang Fang,Huan Xu,Hongtao Wang
TiB 2 reinforced Ti(C,N)-based cermet was produced by the reaction spark plasma sintering of Co, Ni, Ti, C, BN, Mo 2 C, WC, and TaC mixtures. To understand the mechanism of reaction sintering, systematic investigation on the microstructure evolution and displacement variation rule was carried out. In addition, the influence of C/BN molar ratio on the microstructures and performances of cermet was investigated. Except an initially increased pressure, three densification patterns were found. The first method was the Co Ti, Ti Ni, and Ti-BN diffusion reactions, resulting in a shrinkage of 22.06%. The second pattern was the viscous flow and dissolution-reprecipitation, which corresponded to the synthesis of Ti(C,N) and TiB 2 . In this process, the shrinkage ratio was increased by 35.62%. The final densification mainly originated from the viscous flow of metallic binder. It contributed to the transformation of macrovoids into microvoids, and an increased displacement of 30.10%. With the increasing of C/BN ratio, more C atoms diffused into Ti(C,N). Furthermore, core/rim structure-Ti(C,N) and coreless (W,Mo,Ta,Ti)(C,N) were fabricated. However, the microvoids in cermets enhanced. As a result, the hardness and fracture toughness first increased and then decreased. Results from this work are helpful to understand the reaction spark plasma sintering technique, and can enrich the preparation method of cermet.
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CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Jierui Ye,Yuebing Gao,Qingtian Xu,Zhenfu Jin,Guomin Wu,Siqun Wang,Zengkun Cai,Ke Yang,Qiang Wu,Qian Li
Cellulose nanofibrils (CNFs) have widely attracted significant attention due to the excellent mechanical performance, biodegradability, and high surface functionality. However, the high flammability of CNFs commonly restricts their wider application. In this study, the intrinsically flame-resistant holocellulose nanofibrils (HCNFs, which is rich in both cellulose and hemicellulose) were obtained from bamboo under pretreatment using a highly efficient ternary deep eutectic solvent (TDES) and subsequential mechanical homogenization. The phytates and sulfate-containing HCNFs (PHCNFs) displayed nanofibril diameter of 3–5 nm and high aspect ratio of (∼500), and the aqueous suspension exhibited colloidal stability and high transmittance. The PHCNF films exhibited excellent fire resistance, mechanical and optical properties. Compared with raw HCNF, the limiting oxygen index (LOI) of PHCNF-120 film was up to 52.5 %, and the total heat release (THR) and peak heat release rate (PHRR) of PHCNF-120 films were significantly reduced by 92.2 % and 82.4 %, respectively. The flame retardant mechanism was attributed to the synergistic effect of P/N/S in both condensed phase and gaseous phases during the burning process. This work provides a novel, efficient strategy for developing eco-friendly flame-resistant and fireproof holocellulose-based nanomaterials.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 44
·24351-24358
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IF 11.9
Dunren He,Wanyi Nie,Huihui Huang
Hydrovoltaic technology is a promising approach for clean and renewable energy generation, owing to its unique ability to generate electricity from the interactions between nanomaterials and abundant water. However, the output current of hydroelectric generators, which is usually below 1 mA, needs improvement. Here, we demonstrate a large-scale integration of water-graphite hydroelectric generators that can produce an output current of up to 58 mA, surpassing the performance of existing hydroelectric generators, and capable of powering commercial electronics, such as electric fans and full-color liquid crystal display screens. Our results show that this low-cost and scalable hydroelectric generator has the potential to significantly expand the application domain and facilitate the development of clean and renewable energy sources.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
·
2023
·
IF 4.3
Qi Guo,Xiaorong Huang,Yajuan Huang,Zhaowei Zhang,Peiwu Li,Li Yu
Aflatoxin B 1 (AFB 1 ) is a prominent food contaminant known for its high toxicity. Rapid, low-cost, and sensitive detection of AFB 1 is an urgent demand for food safety risk control. In the traditional enzyme-linked immunosorbent assay (ELISA) method for AFB 1 detection, horseradish peroxide (HRP) is high-cost and possesses poor environmental stability. In this study, a direct competitive single-atom nanozymes (SAzymes) -linked immunosorbent assay was developed based on Fe-N-C SAzymes. The proposed methods exhibited excellent sensitivity, rapid detection, fabrication, and low cost. Under the optimal conditions, the limit of detection of the new assay was 3.3 pg mL −1 , with a quantitative relationship between 0.0084 and 0.358 ng mL −1 . In addition, the developed method presented good recoveries in spiked samples, ranging from 84.50% and 103.75%, with coefficients of variation below 10%. Furthermore, the developed detection method showed good consistency (R 2 = 0.9852) with the reference method, liquid chromatography/mass spectrometry (LC-MS/MS). To our knowledge, this is the first report about single-atom nanozymes-based ELISA for AFB 1 determination. This work provides a feasible strategy for the rapid and sensitive detection of food contaminants using SAzymes.
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CARBON
·
2023
·
IF 10.9
Haiqin Zhou,Xiangwei Zhang,Xinchao Zhang,Fang Yuan,Xinlin Wang,Shunlong Yan,Jianbing Wang,Chunquan Li,Zhiming Sun
With the excellent electrical conductivity and unique structure, carbonaceous materials are expected to prepare green catalysts used in sulfate radical based advanced oxidation processes. Nevertheless, most of researches are focusing on artificial synthetic material to date, thus the studies on natural carbon materials call for attention and development. Herein, impregnation-pyrolysis method was employed by adopting the urea as an extrinsic N-dopant under 850 °C to favor C–N configuration for natural microcrystalline graphite (MG). And N element presented as pyridinic N (27.42 %), pyrrolic N (40.08 %), graphitic N (25.86 %) and nitric oxide (6.65 %) in N-doped microcrystalline graphite (NMG). In addition, the catalysis performance of MG, NMG and calcined microcrystalline graphite (CMG) was examined by the degradation of bisphenol A (BPA). The NMG system exhibited high activity in a broad pH range, and acidic conditions promote the reaction rate greatly. Based on quenching tests and electron paramagnetic resonance, the degradation mechanisms comprised radical and nonradical pathway, in which 1 O 2 was the dominant reactive oxidative species (ROS). This study suggested that pyridinic N, pyrrolic N, graphitic N, sp (2)-hybridized carbon structure as well as defects in NMG promoted the generation of ROS, and provides a new insight in natural carbon materials for the fabrication of new eco-friendly and highly efficient PMS activation catalysts.
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