Science Advances
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2023
·Vol. 9
·期 43
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IF 13.6
Wei Zhao,Yiwei Zheng,Meng Jiang,Tingting Sun,Aibin Huang,Lianjun Wang,Wan Jiang,Qihao Zhang
Ionic liquid–based ionogels emerge as promising candidates for efficient ionic thermoelectric conversion due to their quasi-solid state, giant thermopower, high flexibility, and good stability. P-type ionogels have shown impressive performance; however, the development of n-type ionogels lags behind. Here, an n-type ionogel consisting of polyethylene oxide (PEO), lithium salt, and ionic liquid is developed. Strong coordination of lithium ion with ether oxygen and the anion-rich clusters generated by ion-preferential association promote rapid transport of the anions and boost Eastman entropy change, resulting in a huge negative ionic Seebeck coefficient (−15 millivolts per kelvin) and a high electrical conductivity (1.86 millisiemens per centimeter) at 50% relative humidity. Moreover, dynamic and reversible interactions among the ternary mixtures endow the ionogel with fast autonomous self-healing capability and green recyclability. All PEO-based ionic thermoelectric modules are fabricated, which exhibits outstanding thermal responses (−80 millivolts per kelvin for three p-n pairs), demonstrating great potential for low-grade energy harvesting and ultrasensitive thermal sensing.
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SYNTHETIC METALS
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2023
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IF 4.4
Ronghui Guo,Zhimin Ye,Haiyan Zhuang,Qi Zhao,Lai Jiang,Aming Xie
Due to stronger tunability, higher stability, and low production costs, polymeric material-based carbon materials are considered to have the potential to become high-performance electromagnetic wave absorbing (EWA) materials. In this work, polymer-derived carbon is made by pyrolyzing thermoplastic polyimide (TPPI) and thermosetting polyimide (TSPI) at different temperatures. Using Raman and XPS analysis , the graphitization degree and defect content of carbonized TPPI and TSPI are obtained. The reflection loss is calculated by through their electromagnetic parameters. The prepared carbonaceous materials exhibit excellent EWA performance. Specifically, the maximum effective absorption band (EAB max ) of carbonized TSPI at 1500 C can reach 4.1 GHz with thickness of 1.8 mm, and that of carbonized TPPI at 900 C can reach 4 GHz at lower thickness of 1.6 mm. The different structures of TPPI and TSPI result in different degrees of graphitization and defect content at the same temperature, which further leads to differences in their EWA performance. This work provides inspiration for studying the influence of precursor structure on the EWA preformation of carbon materials obtained through pyrolysis.
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ChemistrySelect
·
2023
·Vol. 8
·期 37
·e202301117
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IF 2.1
Mengting Chen,Meihua Zhang,Xiaoshuang Liu,Yingxin Liu
Graphical Herein, we report a highly efficient synthesis of N -arylhydroxylamines through controllable hydrogenation of nitroarenes using hydrazine hydrate as a hydrogen donor over Pt/C catalyst at a low temperature (30 °C). The synthesis of N -arylhydroxylamines through the in-situ hydrogenation of nitroarenes over commercial Pt/C catalyst was investigated. The effects of various reaction conditions including hydrogen donor, solvent, catalyst dosage, temperature and reaction time on the selective hydrogenation of nitrobenzene (NB) to N -phenylhydroxylamine (PHA) were systematically investigated. The results showed that the yield of N -phenylhydroxylamine reached 87.2 % using hydrazine hydrate as hydrogen donor in N,N -dimethylformamide solvent at 30 °C for 60 min. And the catalyst showed no obvious activity loss after a 6-times recycle. Meanwhile, the developed methodology can also transform a range of nitroarenes to the corresponding N -arylhydroxylamines in excellent yields (74–99 %).
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AICHE JOURNAL
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2023
·Vol. 70
·期 1
·e18276
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IF 3.7
Di Hu,Hong Xu,Yongjian Zeng,Lu Lin,Zhiwei Jiang,Kai Yan
The selective hydrogenation of biomass-derived benzoic acid (BA) to cyclohexane carboxylic acid (CCA) is vital to producing fine chemicals from renewable sources. Herein, a novel nitrogen-doped carbon supported bimetallic catalyst (Ni 1 Co 1 /NC) was synthesized via a PVP-assisted method to catalyze the selective hydrogenation of BA to CCA. Compared with the non-doped Ni 1 Co 1 /C and single counterparts, Ni 1 Co 1 /NC exhibited a substantially enhanced activity, with 98.1% yield of CCA. The excellent performance was attributed to the NiCo synergistic effect and N-doped thin carbon layer, which could increase the total proportion of Ni 0 and Co 0 species via donating electrons to Co and thus improve the H 2 adsorption capacity, the hydrogenation activity of aromatic rings in BA and the stability. This work demonstrates a synergetic effect between NiCo bimetal and N-doped thin carbon layer. This would pave the way for the rational design and synthesis of high-performance non-noble catalysts used in BA hydrogenation.
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ELECTROCHIMICA ACTA
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2023
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IF 6.6
Caiyun Xu,Hongwei Yang,Zhizhong Xie,Dan Liu,Hua Zheng,Xi Li,Ruiming Zhang,Haolin Tang,Junsheng Li,Deyu Qu
The rapid growth in energy demands and environmental concerns have drawn great attention to the development of new functional materials for sustainable energy technologies. As an emerging material, mesoporous carbon-based materials exhibit unique properties and have been considered promising candidates for electrochemical hydrogen storage applications. However, pure mesoporous carbon as electrode material may suffer from sluggish electrolyte transportation kinetic and poor hydrophilicity. Two-dimensional layered structure with high exposure area and nitrogen doping, which provides the improved accessibility of ions as well as the hydrophilicity of carbon materials, can cope with these two challenges. Here, the nitrogen-doped layered mesoporous carbon sheets, prepared by the double-hard-template route, were characterized using various technologies and investigated the electrochemically stored hydrogen energy properties. The results exhibit that hydrogen storage can be achieved around 104 mAh g −1 at 100 mA g −1 , and the capacity retention was 85.4% at 2 A g −1 . Moreover, it also displays superior cycling stability with a retention of 98% upon 300 cycles. According to the obtained results, the layered mesoporous carbon sheets demonstrated suitable capacity as a potential and promising active material for hydrogen-proton-related devices.
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ACS Chemical Neuroscience
·
2023
·
IF 5
Mingming Xu,Hong Jin,Wei Ge,Lingbo Zhao,Zhaoliang Liu,Zeyu Guo,Zhen Wu,Jing Chen,Chengjie Mao,Xumin Zhang,Chun-Feng Liu,Shuang Yang
Urine is thought to provide earlier and more sensitive molecular changes for biomarker discovery than blood. Numerous glycoproteins, peptides, and free glycans are present in urine through glomerular filtration of plasma, cell shedding, apoptosis, proteolytic cleavage, and exosome secretion. Urine biomarkers have enormous diagnostic potential, and the use of these biomarkers is a long-standing practice. The discovery of non-urological disease biomarkers from urine is also gaining attention due to its non-invasive sample collection and ease of analysis. Abnormal protein glycosylation in plasma or cerebrospinal fluid has been associated with Parkinson’s disease, however, whether urine with Parkinson’s disease has characteristic glycosylation remains to be explored. Here, we use mass spectrometry-based glycomics and glycoproteomics approaches to analyze urine samples for glycans, glycosites, and intact glycopeptides of urine samples. Reduced abundance of N-glycans was detected at the level of total glycans as well as specific glycosites of glycopeptides. The most abundant N-glycan in urine is S(6)1H5N4F1; S(6)2H5N4 and N4H4F1 are highly present in serum and urine, and 10 biantennary galactosylated N-glycans in the urine of PD patients were significantly decreased. The downregulation of sialylation may be due to the reduction of ST3GAL2. Site-specific N-glycosylation analysis revealed that AMBP, UMOD, and RNase1 have PD-specific N-glycosylation sites. GO and KEGG analysis revealed that N-glycosylation changes may provide clues to identify disease-specific glycosylation biomarkers in Parkinson’s disease.
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COMPOSITES COMMUNICATIONS
·
2021
·
IF 6.617
Congcong Tian,Fan Wu,Wenling Jiao,Xiaoyan Liu,Xia Yin,Yang Si,Jianyong Yu,Bin Ding
The recent outbreak of a coronavirus disease (COVID-19) has posed a great threat to public health and financial system. Most current masks used to prevent the spread of COVID-19 are typically absence of biocidal properties. We designed a novel polymer, polystyrene grafted by 5, 5-dimethylhydantoin and trimethylamine (PSDT), which possesses halamine site and cationic quaternary ammonia salt site. Furthermore, PSDT/PU [email protected] membranes (PSDT/PU NNMs) were obtained by electrospinning technology. Our strategy enables inherent N-halamine and quaternary ammonia salt (QAS) group to be covalently integrated into membranes, realizing the efficient and stable biocidal properties. Meanwhile, the introduction of nanonets endows electrospun membranes with prominent air filtration performance. The resulting membranes exhibit integrated properties of high interception of fine particles (96.7%) and low pressure drop (95.4 Pa). Besides, chlorinated PSDT/PU [email protected] membranes (with active chlorine content of 0.60 wt% and quaternary ammonia salt content of 2.20 wt%) exhibited superior bactericidal (>99.9999%) and virucidal (>99.999%) efficiency in a short time (2 min), which enables chlorinated PSDT/PU NNMs to be served as the filtration material by providing bacterial interception (99.77%) and contact killing against pathogens. The successful synthesis of PSDT/PU NNMs provide innovative insights for exploring filtration materials in a nanonet and biocidal form.
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Results in Chemistry
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2021
·
IF 0
Liu Yang,Hong Zheng,Lian Liu,Wenjie Wu,Shuya Wang
Biomass carbon materials have been widely used as electrode materials for super-capacitors (SC) due to their economic, environmental, and sustainable characteristics. In this work, we proposed that the Sapindus Mukorossi Peel (SMP) was used as a precursor to prepare a Sapindus Mukorossi Peel-based activated carbon material (SMPC) through carbonization and KOH activation. The morphology and structure of SMPC were characterized by various test methods. Cyclic voltammetry (CV), galvanostatic charge–discharge (GCD) and electrochemical impedance spectroscopy (EIS) were used to characterize its electrochemical performance. The results show that SMPC has suitable pore size distribution, a large number of heteroatom functional groups and excellent electrical conductivity. In addition, the amount of activator also has an important influence on the performance of SMPC. When the mass ratio of carbon material to KOH is 1:3, the prepared sample SMPC-3 has the largest specific surface area (SSA) was 1254.5 m 2 /g. Moreover, SMPC-3 also has excellent electrochemical properties, high specific capacitance (at 1 A/g, the specific capacitance can reach 314.5F/g), good cycle stability (at 5 A/g, cyclic charge and discharge 5000 times, the specific capacitance is only lost by 4.2%.), superior rate performance (when the current density is increased from 0.5 A/g to 10 A/g, the specific capacitance retention rate is 80.4%). Assembling SMPC-3 // SMPC-3 into a symmetrical SC shows higher energy density (at 0.1 A/g, the energy density is 6.68 Wh/Kg) and power density (at 5 A/g, the power density is 3250 W/Kg).
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Shasha Wang,Junfeng Miao,Mengshuai Liu,Lihui Zhang,Zhenfa Liu
Novel microporous carbon xerogels (CX-HMTAs) with different morphologies and well-developed porosity were successfully fabricated. The hierarchical pore, surface structure, and nitrogen content could be easily controlled by adjusting the amount of hexamethylenetetramine (HMTA). The samples as-obtained exhibited high micropore volume and large specific surface area, which were applied as supercapacitor electrodes and CO 2 capture materials. The CX-HMTA4 with a moderate concentration of HMTA (0.72 %) afforded the highest CO 2 adsorption capability with 4.21 mmol g −1 at 273 K and 1 bar, and excellent ideal adsorption solution theory (IAST) selectivity with 70 for CO 2 /N 2 capture at 298 K. Moreover, the CX-HMTA4 were simultaneously conducted as a supercapacitor electrode, and gave a maximum specific capacitance of 161 F g -1 and high stability (retained 99.4 % capacity after 1000 cycles) in 6 M KOH electrolyte at 1 A g -1 , showed a great advance when compared with most reported benchmark carbon materials. The multifunctional porous carbon materials presented herein were facilely prepared without any activation, exhibiting considerable potentials for large-scale gas adsorption/separation and electrochemical energy storage.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Ying Han,Kemin Zhang,Qingjie Lu,Zhao Wu,Jun Li
Since iron (Fe) was first proven to have a strong reduction ability, it has been successfully applied to remove pollutants from water. In this study, nickel hydroxide (Ni(OH) 2 ), a catalyst commonly used in hydrogen evolution reactions, was added to improve the activity of Fe to remove N- nitrosodimethylamine (NDMA). The results showed that with the increasing Ni(OH) 2 dosages, the reactions accelerated. The NDMA removal rates increased when the pH value was 6 or 7. Further, when the dissolved oxygen concentration was in the range of 0–12.0 mg∙L −1 , it had little effect on the Fe/Ni(OH) 2 system, and all the reactions obeyed pseudo-first-order kinetics. 1,1-dimethylhydrazine and dimethylamine were formed during NDMA degradation. The capture of active substances and electron spin resonance method confirmed that the main active species were active hydrogen atoms , which participated in the removal of NDMA. Ni(OH) 2 acting as a catalyst was confirmed using wide-angle X-ray diffraction, X-ray photoelectron spectroscopy and Ni 2+ dissolution. Further, catalytic hydrogenation was proposed as the main removal mechanism as Ni(OH) 2 promotes the corrosion of Fe and dissociation of water, thereby generating more active hydrogen atoms. In addition, Ni(OH) 2 may activate both Fe and NDMA. This technique could be employed as an alternative for NDMA reduction and expand the application field of Ni(OH) 2 .
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Journal of Physical Chemistry C
·
2021
·
IF 4.126
Pengfei Yao,Jing Cao,Xue Gong,Ce Han,Mingbo Ruan,Ping Song,Weilin Xu
The development of catalysts free of platinum-group metals with a high performance for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells is a grand challenge. Herein, we report zeolitic imidazolate framework-8-based Co, N, and S tridoped carbon frameworks (Co–N–S CFs) with high ORR catalytic activity and remarkable durability in an alkaline medium. Results indicate that the high ORR performance of the Co–N–S CFs could be attributed to the unique 3D structure of carbon frames, the synergistic effect among Co, N, and S, and its high electron conductivity. It is also found that the N and S doped heteroatoms can anchor Co atoms by forming CoNx and CoSx active sites for a highly efficient ORR. The results obtained here can help in the design and understanding of the cost-effective highly active Pt-free electrocatalysts.
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COMBUSTION AND FLAME
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2021
·
IF 4.185
Wang Li,Jiu-Zhong Yang,Long Zhao,Dan Yu,Zhen-Yu Tian
With biofuels market expanding, amines, as an important compound class in biofuels, are attracting increasing attention. The pyrolysis of n-propylamine (NPA) was studied in a flow tube using tunable synchrotron photoionization and molecular-beam mass spectrometry techniques. 28 and 30 species, including nitrogenous compounds and hydrocarbons, were identified and quantified at 30 and 760 Torr, respectively. 1,3-Cyclopentadiene, 1,4-pentadiene, 2-methyl-1,3-butadiene and benzene, were newly detected compared with previous studies of methylamine and ethylamine. HCN, NH 3 , N 2 and methanimine were detected as the dominant nitrogenous products. Moreover, minor aliphatic and unsaturated amines were also identified, such as methylamine, ethylamine and acetaldimine. Ethylene achieved at the highest level among hydrocarbon products. With the pressure increasing, the onset temperature of NPA pyrolysis shifts towards low temperature region and NPA decomposes faster. A comprehensive detailed kinetic model involving 405 species and 2668 reactions was developed with reasonable predictions. According to rate-of-production analysis, H-abstractions, especially at C α position of NPA, are the major consumption pathways of NPA. In addition, unimolecular reaction breaking C α -C β bond is the important consumption channel of NPA at 30 Torr, while its positive effect is seriously weakened at 760 Torr. The H-abstraction at C α (NPA+ H CH 3 CH 2 CHNH 2 +H 2 ) plays a leading role for NPA consumption at 760 Torr. The reactions, CH 3 +CH 3 =C 2 H 5 + H and CH 3 CHCHNH 2 + H CH 2 CHCHNH 2 +H 2 , tend to present inhibiting effects on NPA consumption at 30 and 760 Torr, respectively. These results could provide a theoretical basis for further combustion kinetic studies of biofuels and amine fuels.
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