Advanced Sustainable Systems
·
2022
·Vol. 6
·期 3
·2100380
·
IF 6.737
Zhengyi Li,Hu Li,Song Yang
Catalytic upgrading of CO 2 into value-added chemicals to build the excess carbon cycle is of great significance. In this work, carboxylate-functionalized zeolitic imidazolate framework (F-ZIF-90) with good crystallinity and porosity is constructed from ZIF-90 and employed as a robust heterogeneous catalyst to boost the reductive N -functionalization of various amines with CO 2 to furnish N -formyl compounds (up to 99% yield) in the presence of PhSiH 3 under an ambient environment. The imidazole carboxylate species ( COO - ) can not only activate hydrosilane and CO 2 to form the key intermediate formoxysliane but also activate amines to participate in the N -formylation reaction to obtain the target product. Moreover, it can enhance the catalyst capture and exchange ability toward ambient CO 2 . The powerful adsorption capacity of the F-ZIF-90 catalyst toward CO 2 is conducive to elevating CO 2 concentration around the active species. Theoretical calculations show that the carboxylate-mediated conversion path undergoes the transition state of hydrosilane activation with a relatively lower energy barrier (Δ G = 26.9 kcal mol –1 ). F-ZIF-90 exhibits good thermochemical stability with no obvious activity attenuation after repeated use 5 times. This strategy opens a new avenue based on ZIFs to develop heterogeneous catalysts for reductive upgrading of CO 2 .
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Wei Sun,Kang Guo,JinChen Fan,Yulin Min,Qunjie Xu
In this paper, we have adopted a simple and etching-free method to prepare mesoporous carbon spheres in one step. Selenium can be deposited in the internal cavity, which can avoid pulverization due to the combined effect of volume expansion and a solid–electrolyte interphase (SEI) film while charging and discharging. Therefore, the as-prepared selenium and nitrogen codoped mesoporous carbon nanosphere (Se@NMCS) composites can deliver an outstanding sodium-storage performance of 336.6 mAh g–1 at a present density of 200 mA g–1 and great long-cycling performance. For a further understanding of the Na+ storage mechanism of the Se@NMCS anode in sodium-ion batteries (SIBs), the phase evolution of the Se@NMCS anode has been explored during the charge/discharge process by conducting in situ Raman investigation.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2015
·
IF 2.999
Lin Chen,Huibo Wang,Chengzhan Liu,Xianchun Liu,Shuangxi Xing
Highly dispersible copper nanoparticles (CuNPs) anchoring on the N-doped carbon films are achieved by pyrolyzing urea, citric acid and copper nitrate in one pot. The presence of the CuNPs and the N-doped carbon film is investigated by transmission electron microscopic, X-ray diffraction, X-ray photoelectron and Raman spectra. The citric acid is used as a carbon source to support the as-synthesized CuNPs and the urea takes a role as a nitrogen source to dope into the carbon structure and localize the CuNPs with a separated state. Such an N-doped carbon film with well-dispersed CuNPs on its surface presents an excellent catalytic performance and stability via using the reduction of 4-nitrophenol by NaBH 4 as a model reaction.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Cong Huang,Lirong Zheng,Wenshuai Feng,Aimin Guo,Xiaohui Gao,Zhen Long,Xiaoqing Qiu
In recent years, metal isolated site catalysts with the high exposure and maximized availability of metal species provide a new route to boost the oxygen reduction performance. However, in the absence of clusters and nanoparticles, the synthesis of this catalyst with metal high-loading, especially for copper, is still a big challenge. In this work, a metal isolated site catalyst with high copper content (1.12 wt %), copper isolated sites anchored on N-doped carbon materials (donated as Cu ISs/NC-1000), was prepared by the pyrolysis of copper acetylacetone within the metal–organic framework (ZIF-8) at 1000 °C. The successful preparation of products can be demonstrated by high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption spectra. With the merits of the atomically dispersed surface metal atoms and abundant ORR-favored copper active sites, the present Cu ISs/NC-1000 exhibits an excellent ORR electrochemical activity with a half-wave potential of 0.855 V (vs RHE) and a limiting current density of 5.2 mA cm–2 in the electrochemical tests, superior to the results from commercial Pt/C and previously reported Cu-based materials. For the durability, the negligible activity decay after 10,000 continuous potential cycles and good resistance to methanol crossover can be noted. The outstanding catalytic activity from the present Cu ISs/NC-1000 demonstrates the superiority of metal isolated sites as electrocatalytic centers.
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ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Jieting Ding,Shan Ji,Hui Wang,Vladimir Linkov,Hengjun Gai,Fusheng Liu,Quanbing Liu,Rongfang Wang
Water electrolysis offers a promising approach toward future sustainable energy mix utilizing hydrogen as energy carrier. Bifunctional catalyst which is active in both oxygen and hydrogen evolution reactions can significantly enhance total electrochemical water splitting efficiency and simplify electrolysis systems. In this study, nitrogen doped nickel-containing porous carbon networks were prepared to fulfill this role. Peptone was used as carbon and nitrogen source during the synthesis and NaCl presence as a template resulted in the formation of open mesopores interconnected by thin carbon sheets with nanosized Ni particles encapsulated in the carbon matrix. A low onset potential of 53 mV and a charge transfer resistance of 3.8 Ω with excellent cycling stability were demonstrated when the optimized catalyst Ni-2 was applied in HER. It was also shown that Ni-2 onset potential, charge transfer resistance, and durability in OER were comparable to those of a commercial RuO2 catalyst. During the electrolysis study conducted at 10 mA cm–2, Ni-2 maintained a cell voltage of 1.63 V with remarkable stability during 25 h operation.
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RSC Advances
·
2014
·Vol. 4
·期 29
·14979-14984
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IF 3.708
Meng Deng,Bo Su,Hui Zhang,Yuxiu Liu,Qingmin Wang
A concise and efficient enantioselective strategy to synthesize two typical phenanthroindolizidine alkaloids, 14-hydroxyantofine and antofine, was developed, featuring an asymmetric deprotonation/diastereoselective carbonyl addition sequence during which the formation of a chiral C-13a center and connection of pyrrolidine and phenanthrene moieties were achieved efficiently in one step. The absolute configuration of the C-13a stereocenter can be delicately controlled by using different enantiomers of sparteine, both of which are commercially available.
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CELLULOSE
·
2024
·Vol. 31
·期 8
·5263-5280
·
IF 4.9
Han Qiuxia,Xu Yanmeng,Zhao Qian,Wang Shiwei,Zhang Chunzhe,Zhang Qiang,Wang Fei,Bai Yu,Chen Yong
The study reports a tactic for superior antibacterial performance on cotton via synergism of complementary functionalities of quaternary ammonium salt and malonylurea-based N -chloramine combined in a silane. Knoevenagel Condensation between 4-(chloromethyl)benzaldehyde and malonylurea formed a product whose chloromethyl group was used to quaternize tertiary amine of N , N -dimethylethanolamine. The O − H of the quaternization product was subsequently alcoholyzed with Si − H of trimethoxysilane. The methoxysilyl groups of the alcoholysis silane were hydrolyzed to silanol ones that condensed with either their own kind or hydroxy groups of cellulose to polymerize into a crosslinked polysiloxane finishing on cotton. Upon chlorination of malonylurea-based N − H bonds, each repeating unit of the polysiloxane has one quaternary ammonium salt and two imide N -chloramine sites. Antibacterial assays against Staphylococcus aureus and Escherichia coli proved that the synergism of quaternary ammonium salt and N -chloramine, a higher efficacy and a broader spectrum arising from their complementary elimination mechanisms and physiochemical features. Biocidal stability and rechargeability of the polysiloxane finishing were both promising due to the robust and hydrophobicity of silicone backbone and the sturdy cyclic N -chloramine. This research presented a general approach for generation of super biocidability on substrates that can react with hydroxy group using silanes to carry complementary functionalities. Graphical abstract
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BIOORGANIC CHEMISTRY
·
2025
·
IF 4.7
Ruobin Sun,Qipeng Yan,Wenhao Deng,Pengcheng Chen,Dan Wu,Pu Zheng
Achieving enzyme catalysis at high substrate concentrations is a substantial challenge in industrial biocatalysis, and the role of glycosylation in post-translational modifications that modulate enzyme substrate inhibition remains poorly understood. This study provides insights into the role of N -glycosylation in substrate inhibition by comparing the catalytic properties of d -lactonohydrolase ( d -Lac) derived from Fusarium moniliforme expressed in prokaryotic and eukaryotic hosts. Experimental evidence indicates that recombinant d -Lac expressed in Pichia pastoris ( Pp Lac-WT) exhibits higher hydrolysis rates at a substrate concentration of 400 g/L, with reduced substrate inhibition and enhanced stability compared to the recombinant d -Lac expressed in Escherichia coli ( Ec Lac-WT). Mutant Pp Lac-M1 achieves a conversion rate of 40 % at a substrate concentration of 400 g/L, with a space–time yield of d -pantoic acid reaching 91.1 g/L/h. Proteomics analysis reveals that residues N29 and N278, located approximately 10–20 Å from the active site undergo N -glycosylation in Pp Lac-WT. Using microsecond-scale molecular dynamics simulations and Markov state models, we elucidate the effects of glycosylation on the conformational flexibility of two key loops at the entrance of the binding pocket. Specifically, the loops in Pp Lac-WT can transition between open and closed states, whereas those in Ec Lac-WT tend to remain open. In high substrate concentration conditions, the open state causes congestion, leading to substrate inhibition. Shortest-path map analysis confirms that substrate entry is dynamically controlled by residue N29 on the loops surrounding the active site. Our findings enhance the understanding of the effects of glycosylation on enzyme conformational dynamics and provide insights into mitigating inhibition at high substrate concentrations.
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PubMed
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Peng Wei,Xin Ye,Jianhua Jiao,Fan Wu,Haodong Zhang,Shaoyang Wu,Shanshan Lv,Qirui Liang,Yurong Ren
Iron phosphide (FeP) has garnered significant attention due to its abundant iron reserves, low cost and impressive hydrogen evolution reaction (HER) activity. Nevertheless, sluggish charge transport, large particle size and poor oxygen evolution reaction (OER) activity make it still difficult to meet the desired practical applications. As we know, heterogeneous element doping, porous two-dimensional structure design, and nanoconfinement control can effectively improve the mass/charge transfer rate and expose more active sites. Hence, ultra-small bimetallic iron-cobalt phosphide nanoparticles encapsulated and dispersed in two-dimensional nitrogen-doped carbon nanosheet (FeCoP@NC) catalysts were successfully constructed. The optimized FeCoP@NC shows outstanding electrocatalytic stability and activity toward OER and HER under alkaline conditions. The overall water splitting performance was further measured by using FeCoP@NC as both anode and cathode, which also delivers good performance indicators. This work provides a new perspective and potential value for the rational design of non-precious metal bifunctional catalysts.
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Jiayi Qu,Yujun Guo,Xingtai Chen,Xiaoning Wang,Davoud Dastan,Xi-Tao Yin,Xiaoguang Ma
Dy 2 O 3 -CdS nanomaterials was firstly prepared by a one-step hydrothermal method for the rapid detection of n-butanol. In comparison with the sensor solely based on CdS, the integrated gas sensitivity performance of the sensor S 2 (containing 10 mol % Dy 2 O 3 ) for n-butanol was significantly improved, with a response value of up to 130, 3.25 times higher than that of the pristine CdS for 100 ppm n-butanol gas at an optimal operating temperature of 200 °C, this represents a substantial enhancement in the sensitivity of n-butanol detection, outperforming many existing sensing materials. Secondly, the sensor not only demonstrates excellent selectivity and long-term stability towards n-butanol but also enables highly precise detection within the wide concentration range of 5-300 ppm, Additionally, it possesses a fast response/recovery time of 25/18 s, significantly improving the detection efficiency. After a sequence of characterization utilizing XRD (X-ray diffraction), SEM (scanning electron microscope), TEM (transmission electron microscope), XPS (X-Ray photoelectron spectroscopy), the study reveals that the superior gas-sensing performance is attributed to the formation of n-n type heterojunctions, the interconnection of CdS nanomicrospheres by Dy 2 O 3 nanorods that facilitates gas transport, and the unique 4f electrons of Dy 2 O 3 . These findings provide new insights into the design of high-performance gas sensors, distinguishing this work from previous studies and making it a valuable contribution to the field of n-butanol detection.
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CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Qingsong Luo,Yan Chen,Changhao Feng,Shuang Gao,Tianyu Lan,Qiyuan Fu,Runduo Teng
For applications in environmental protection, industrial production, and personal health monitoring by breath exhalation, the sensitive and selective detection of n-butanol is of extreme importance. An n-butanol gas sensor has been developed utilizing LaFeO 3 nanofibers doped with Er 3+ by an electrospinning technique. Compared to the pure sample, the gas sensor shows an improved response of 58.97 to 30 ppm n-butanol, which was boosted by 5.99-fold due to the smaller average grain sizes (21.2 nm), porosity of the nanofiber, and abundant chemical-absorbed oxygen species (38.5%) at an Er doping level of 3 at%. It has excellent selectivity to n-butanol, a fast response/recovery time (17 s/27 s), superior stability during 30 days, and a low detection limit (100 ppb), which indicates that Er-doped LaFeO 3 nanofibers have excellent sensing capabilities for real-time n-butanol detection.
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TOXICOLOGY LETTERS
·
2020
·
IF 3.569
Jianxin Ye,Kangnan Zhang,Xindi Yuan,Haosen Ji,Miner Hu,Tongliang Huang,Ren-Shan Ge
Di -n- hexyl phthalate (DNHP) is commonly used as a plasticizer. However, whether DNHP influences Leydig cell development during puberty remains unexplored. In this study, DNHP (0, 10, 100, and 1000 mg/kg) was administered via gavage to 35-day-old male Sprague-Dawley rats for 21 days. Serum levels of testosterone, luteinizing hormone, follicle-stimulating hormone, Leydig cell number, the expression of Leydig and Sertoli cell genes and proteins were investigated. DNHP significantly increased serum testosterone levels at 10 mg/kg but lowered its level at 1000 mg/kg. DNHP significantly increased luteinizing hormone levels at 1000 mg/kg without affecting follicle-stimulating hormone levels. DNHP increased Leydig cell number at all doses but down-regulated the expression of Lhcgr , Hsd3b1 , Hsd17b3 , and Hsd11b1 in Leydig cell per se at 1000 mg/kg. DNHP elevated phosphorylation of ERK1/2 and GSK-3β at 10 mg/kg but decreased SIRT1 and PGC-1α levels at 1000 mg/kg. In conclusion, DNHP exposure causes Leydig cell hyperplasia possibly via stimulating phosphorylation of ERK1/2 and GSK-3β signaling pathways.
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PubMed
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