APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Wenjie Xue,Hongxia Liu,Binbin Zhao,Lixia Ge,Shuai Yang,Minghuang Qiu,Jiong Li,Wei Han,Xinqing Chen
N-ethylcarbazole (NEC) has been considered one of the most prospective liquid organic hydrogen carriers (LOHCs) for hydrogen storage. However, designing single catalyst capable of driving both hydrogenation of NEC and dehydrogenation of dodecahydro-NEC (12 H-NEC) is of a big challenge. Herein, we develop an atomic-dispersion of Rh with the Co nanoparticles (NPs) to form a Rh 1 Co structure maximizing the Rh utilization, which boosts the reversible (de)hydrogenation of NEC, and enables multiple cycles of reversible hydrogen uptake and release. Significantly, a low temperature of 90 °C is realized for the complete hydrogenation (100%), representing one of the lowest temperatures yet reported for the total hydrogenation of NEC. The remarkable catalytic performance of Rh 1 Co catalysts is the result of the optimal electronic structure between atomic-dispersion of Rh and Co NPs confirmed by structural characterizations and density functional theory (DFT) calculations, which allowed fast interfacial electron transfer to intermediates.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Wenhan Jia,Hao Wu,Yunxin Zheng,Ziyi Liu,Gaotuo Cai,Jianfeng Wen,Guanghui Hu,Tao Tang,Xinyu Li,Li Jiang,Zhiyong Wang,Ming Li,Haifu Huang
Herein, we demonstrate the enhanced pseudocapacitive performance of a MoS2-based flexible supercapacitor by the co-doping strategy of cations and anions. The MoS2 nanosheet arrays on carbon cloth are directly doped with N and Co atoms through a simple hydrothermal process. The obtained cation and anion co-modified MoS2 (N-Co-MoS2) shows improved electron transport efficiency and enhanced active sites for MoS2. According to the first-principles calculations, N-Co-MoS2 has a unique band structure and high electrical conductivity. As expected, N-Co-MoS2 shows higher capacitive performance with 5072.5 mF cm–2 and a better cycle life (retaining 100% capacitance after 10,000 cycles) than pure MoS2. Furthermore, a solid-state flexible N-Co-MoS2 supercapacitor device is fabricated to demonstrate excellent mechanical stability with a specific capacitance of 3236 mF cm–2 and a stable cycle capacitance of 75.56% after 5000 cycles. In our work, we have provided a reference for preparing MoS2-based materials with good supercapacitive performance.
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APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Yu Liu,Zhichao Miao,Manfen Liang,Jie Zhang,Jinping Zhao,Leilei Xu,Jin Zhou,Shuping Zhuo
Electrocatalysis of CO 2 to CO is not only conducive to the artificial carbon cycle, but also green and efficient technology for producing chemicals. In consideration of the practical application, the novel strategy for large-scale preparation of catalyst has great potential to be developed. Herein, a facile one-step approach was developed for constructing a group of N -doping carbon-encapsulated metal catalysts (M@N C (M = Fe, Co, and Ni)) for CO 2 electroreduction to CO. In addition, the impact of metal on catalytic performance was detailedly researched. Specifically, the Ni@N C catalyst achieves an excessive CO Faraday efficiency (FE CO ) (>90 %) on a broad achievable potential window of − 0.67 V to − 0.97 V vs RHE in the H-type cell. The optimal catalyst attains a FE CO of 98 % at − 0.57 V vs RHE and an industrial-relevant current density of 430 mA cm −2 at − 1.07 V vs RHE in the flow cell. This work provides a facile way to fabricate catalyst on a large scale with preeminent performance for industrial CO 2 electroreduction to CO.
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Polymers
·
2022
·Vol. 14
·期 23
·5135
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IF 4.967
Xu Han,Yun Tao,Chao Xu,Yicong Deng,Zisen Meng,Zhenhao Dou,Peng Wang,Quan Feng
Hemin possesses great potential in eliminating organic pollutants due to its mild reaction condition, light-harvesting efficiency, and environmental friendliness. However, it has drawbacks such as being easy to aggregate and hard to recycle, and poor stability should be improved in practical application. Herein, the subject developed an electrospinning approach to enable the hemin particulates to be immobilized onto polyacrylonitrile (PAN) nanofibers stably. Hydrogen peroxide (H2O2) was adopted as an oxidant in the system to simulate the enzymatic catalysis of hemin in an organism. Scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), UV-Vis diffuse reflection spectroscopy (DRS), and electron spin resonance spectroscopy (ESR) analysis was employed to discuss the morphology, structure, and mechanism of the prepared n-hemin/PAN nanocomposite membranes, and 0.02 mmol L−1of the rhodamine B (RhB) removal activity in different conditions was also verified with these membranes. The kinetic studies showed that n-hemin/PAN nanocomposite membranes maintained excellent properties both in adsorption and degradation. Around 42% RhB could be adsorbed in the dark, while 91% RhB decolorized under xenon lamp irradiation in 110 min, suggesting the catalytic performance of n-hemin/PAN was greatly driven by light irradiation. Differing from the axial coordinated hemin complexes, n-hemin/PAN would catalyze hydrogen peroxide into •OH radicals rather than •OOH and high-valent metal-oxo species. This work provides an effective way to support hemin as nanocomposite membranes, in which the molecular interaction between polymer and hemin made their light adsorption an obvious red shift.Keywords:polyacrylonitrile;hemin;photocatalysis;enzyme-like catalysis;electrospinning
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RADIATION PHYSICS AND CHEMISTRY
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2023
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IF 2.9
Junhua Luo,Li Jiang,Long He,Liang Zhou
The secondary nuclear decay method was applied for the cross-section measurement of the 81 Br(n,2n) 80m Br reaction. As a result, the cross-sections of the 81 Br(n,2n) 80m,g Br reactions with a detailed uncertainty propagation and their isomeric cross-section ratios σ m /σ g were obtained at four neutron energies within the range from 13 to 15 MeV by applying an activation and off-line γ-ray spectrometric technique. The Br-based samples and Nb-based monitor foils were activated together to determine both the reaction cross-sections and the incident neutron flux . The neutron beam was formed via the 3 H( d , n ) 4 He reaction. The cross-sections were also calculated by using a theoretical nuclear model code TALYS-1.95 with different options of level density at neutron energies varying from the reaction threshold to 20 MeV. The extracted results were analytically discussed and compared with the corresponding theoretical and evaluated data from the published works in the literature.
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LUMINESCENCE
·
2023
·Vol. 38
·期 2
·188-195
·
IF 2.9
Xin Wang,Changjian Zhu,Xuerong Yan,Sijie Cheng,Yong Zhang
N-doped carbon dots (N-CDs) were synthesized from L -glutamine and triethanolamine using a one-step hydrothermal method. The N-CDs emitting blue fluorescence had selective responses to tetracyclines (TCs) and could be used as a fluorescent probe to realize the quantitative detection and qualitative analysis of TCs. A method for the determination of TCs using the N-CDs in actual samples was successfully established. The recovery rate was maintained at 97.50–105.60%, and the relative standard deviation (RSD) was less than 3%. In addition, TCs can be visually distinguished using filter paper by the different fluorescence colours (light green, dark blue, and yellow-green) of the N-CDs/TCs system under ultraviolet light. This study provides a relatively simple method to detect and identify TCs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jiarun Cheng,Chaojie Lyu,Hangren Li,Jiwen Wu,Yue Hu,Bin Han,Kaili Wu,Mirabbos Hojamberdiev,Dongsheng Geng
An original strategy was reported to manipulate ORR selectivity of N-doped hollow mesoporous carbon spheres (N-HMCS) via heteroatom (P and S) doping. Heteroatom doping can not only modulate electronic structure of N-HMCS and proportion/configuration of doped N, but also regulate ORR pathway. Specifically, rich-graphitic N sites and electron-rich C–P bond domains in N,P-HMCS act as electron donors, making *OOH more unstable and easier to desorb into H 2 O 2 . This severely distorts the sp 2 lattice of graphene, catalyzing a two-electron ORR synergistically. Conversely, a strong interaction between electron-deficient C–S bond domain and *OOH intermediate due to the introduction of highly electronegative S hinders the desorption of *OOH, leading to the breakage of the O–O bond and promoting four-electron ORR along with the rich-pyridinic N receptor site. The reaction activity and kinetics mechanism present a positive correlation with proportion of graphitic N, revealing graphitic N is the primary active site with a much faster electron transfer capacity.
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International Journal of Applied Ceramic Technology
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2023
·
IF 2.1
Mengwen Zhang,Na Cao,Fanyu Meng,Lutong Yang,Binyang Jiang,Jinsheng Li,Lei Fan,Shoulei Yang
High-toughness Al 2 O 3 –Ti(C,N) composites reinforced by cBN particles were prepared by the new oscillating pressure sintering technique. The density, phase, and microstructure evolution of the Al 2 O 3 –Ti(C,N)-cBN composites sintered at different temperatures were studied, and their effects on the mechanical properties were investigated. The results show that when the sintering temperature increases from 1300 to 1500°C, the heat preservation time shortens, whereas the density and interface bonding strength of the composites increase. In addition, cBN particles can play the role of crack bridging and be pulled out when the composites fracture, improving the toughness of the Al 2 O 3 –Ti(C,N)–cBN composites. However, when the sintering temperature further rises to 1600°C, a new phase of TiB 2 forms, and the solid solubility of C and N in Ti(C,N) increases, leading to a decrease in density and mechanical properties. As a result, when the Al 2 O 3 –Ti(C,N)–cBN composite is sintered at 1500°C, its mechanical properties reach the maximum values of 21.5 GPa, 5.7 MPa m 1/2 , and 731 MPa for hardness, fracture toughness, and flexural strength, respectively.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 26
·期 4
·3263-3273
·
IF 3.3
Ziwei Zhai,Bofeng Zhang,Yutong Wang,Guozhu Liu
Based on the disturbance of electronic density, nitrogen-doped nanocarbons show promising properties to anchor metal clusters. However, precisely regulating the coordination mode between N species and the active site remains challenging. Herein, we rationally designed three N types (graphitic N, pyridinic N and pyrrolic N) in nanocarbons to anchor Pt clusters for the benchmark propane dehydrogenation. The specific activity of the pyridinic-N-doped catalyst was 147.54 molC3H6 molPt−1 h−1 at 550 °C, which was 1.3 times higher than those of graphitic- and pyrrolic-N-doped catalysts. Unlike the regular tetrahedron Pt cluster in the graphitic-N catalyst or the distorted three-layered Pt cluster in the pyrrolic-N catalyst, the Pt cluster in the pyridinic-N catalyst was an inverted tetrahedron, which increased the contact degree without geometric repulsion towards C–H bond scission. The geometric parameters of detached H and C atoms in the methylene group for the pyridinic N catalyst was decreased to strengthen the C–H bond scission. After CH3CHCH3* adsorption, the Bader charge of the Pt active site also became highly positive, which tailored the d-band center closer to the Fermi level and provided more vacant orbitals for C–H bond breakage. Therefore, pyridinic N in nanocarbons is promising to anchor small-sized Pt for alkane dehydrogenation in terms of geometric and electronic effects.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Yi-Fan Xue,Jie Feng,Jin-Yao Ma,Wen-Ying Li
C–N bond breaking is a difficult but crucial step in the quinoline removal of coal-based liquids. Noble metal catalysts have higher C–N bond breaking activity, but their surface bond breaking mechanism is unclear. Atomic layer deposition creates more metal-oxide sites and generates different active species, which facilitates the mechanism study. For this reason, we used atomic layer deposition to deposit TiO 2 on the catalyst surface and suggested a more complete C–N bond breaking mechanism in this study. The particle size and pore structure of the catalyst did not change significantly after the deposition, and the hydrogen adsorption was reduced when there were too many layers deposited and the surface Pt sites were occupied to a high degree. TiO 2 is extremely susceptible to reduction to Ti 3+ under hydrogen, and can change the nature of the electron density of Pt through oxygen vacancies, creating Ti 3+ -Pt δ− sites that are prone to protonation reactions. That means, the occurrence of these protonation reactions not only easily breaks the C–N bond, but also accelerates the rate of C–N bond cleavage due to the increased H coverage on the surface of the xcTi-PtAl catalysts. And the Ti 3+ -Pt δ− sites in catalyst had a stronger adsorption effect on the nitrogen-containing compounds, which in turn lowered the energy barriers of bond cleavage. It is concluded that protonation is a necessary step before the C–N bond can be broken. The subsequent steps were showed by the DFT calculations that the nitrogen-containing compounds adsorbed on the Ti 3+ -Pt δ− sites undergo β-H fracture after the protonation reaction, with the elimination reaction cleaving the C–N bond. The xcTi-PtAl catalysts by atomic layer deposition of Ti not only improve the C–N bond breaking performance, but also improve bond breaking stability by a factor of four compared to the Pt/Al 2 O 3 catalysts.
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Frontiers in Chemistry
·
2023
·
IF 5.5
Jing-Jing Xu,Jiao Luo,Heng Xi,Jin-Bu Xu,Lin-Xi Wan
A series of novel N -aryl-debenzeyldonepezil derivatives ( 1–26 ) were designed and synthesized as cholinesterase inhibitors by the modification of anti-Alzheimer’s disease drug donepezil, using Palladium catalyzed Buchwald-Hartwig cross-coupling reaction as a key chemical synthesis strategy. In vitro cholinesterase inhibition studies demonstrated that the majority of synthesized compounds exhibited high selective inhibition of AChE. Among them, analogue 13 possessing a quinoline functional group showed the most potent AChE inhibition effect and significant neuroprotective effect against H 2 O 2 -induced injury in SH-SY5Y cells. Furthermore, Compound 13 did not show significant cytotoxicity on SH-SY5Y. These results suggest that 13 is a potential multifunctional active molecule for treating Alzheimer’s disease.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2023
·Vol. 415
·期 23
·5575-5588
·
IF 4.3
Liu Yuanyuan,Han Yutong,Zhu Wenjie,Luo Qingming,Yuan Jing,Liu Xin
Glycosylation is one of the most common types of post-translational modifications in mammals. It is well known that N-glycans play a key role in cell adhesion, differentiation, synapsis, and myelination during the development of the mammalian central nervous system (CNS). Neuropathological symptoms (such as epilepsy and Alzheimer’s disease) are usually accompanied by N-glycosylation changes. In this study, we extracted N-glycan chains from eight regions of the mouse brain, and combined high-throughput, high-resolution matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF/MS) with the Fmoc N-hydroxysuccinimide ester (Fmoc-OSU) derivatization method to improve the sensitivity of glycan detection to characterize the total N-glycans in the mouse brain. A total of 96 N-glycan moieties were detected. An exhaustive examination of the relative abundance of N-glycans, coupled with a comparative analysis of differences, has uncovered discernible variations of statistical significance, including high mannose, fucosylated, sialylated, and galactosylated N-glycans. According to our investigations, a thorough and regionally specific cartography of glycans within the brain can facilitate the investigation of glycan-mediated mechanisms related to both the developmental trajectory and functional output of the brain. Additionally, this approach may serve as a basis for identifying potential biomarkers that are relevant to various brain-associated pathologies. Graphical Abstract
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