Catalysts
·
2022
·Vol. 12
·期 12
·1525
·
IF 4.501
Sai Che,Na Ta,Fan Yang,Yulong Yang,Yongfeng Li
Rational design and construction of cost–effective electrocatalysts for efficient hydrogen production has attracted extensive research attention worldwide. Herein, we report the construction of a transition metal selenide/carbon composite catalyst featuring uniform NiSe nanoparticles anchored to single Ni atom doped porous carbon structure (NiSe/Ni–N–C) via a facile one–pot pyrolysis of low–cost solid mixtures. NiSe/Ni–N–C exhibits remarkable catalytic performance towards hydrogen evolution reaction (HER) in 1.0 M KOH, requiring a low overpotential of 146 mV to reach a current density of 10 mA cm−2. The unique carbon layer encapsulation derived from the enwrapping of fluid catalytic cracking slurry further renders NiSe/Ni–N–C excellent for long–term durability in electrolyte corrosion and nanostructure aggregation. This work paves the way for the design and synthesis of highly efficient composite HER electrocatalysts.Keywords:NiSe nanoparticle;single atom catalyst;interfacial electronic engineering;hydrogen evolution reaction
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ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Zhixin Chen,Yijie Wang,Liming Hu
Thermal desorption technology can effectively remediate fuels-contaminated clayey soil. However, the microscopic mechanism for the contaminant desorption on clay is still unclear, especially with the existence of water on clay surfaces. In this study, a combination method including TGA experiments, multi-phase and multi-component kinetic models, and MD simulation was proposed to reveal the thermal desorption mechanism of n -dodecane in unsaturated clay. Results showed that the thermal desorption behavior of the free nonaqueous phase liquid (NAPL) and the adsorbed phase of n -dodecane or water could be identified by the multi-phase and multi-component kinetic models based on the desorption process rate obtained by thermogravimetric analysis (TGA) experiments. The activation energy of the NAPL phase (49–69.9 kJ/mol) was lower than the adsorbed phase (90 kJ/mol). The activation energy of the NAPL phase had the same linear relationship with its mass on kaolinite and montmorillonite , while adsorbed phase only existed on the kaolinite surface. MD simulation showed that water demonstrated competitive adsorption with n -dodecane on montmorillonite surfaces and prevented the formation of the adsorbed phase while having little influence on the n -dodecane adsorption on kaolinite surface, which agrees well with the kinetic analysis of the TGA experiments. With the combination of macroscopic experimental analysis and microscopic molecular simulation, it can be concluded that the mass of the NAPL phase limited the desorption behavior, while the interaction between the clay mineral surface and n -dodecane was the key factor that dominated the thermal desorption behavior of the adsorbed phase. The presented results provide new insight into the desorption mechanism of hydrocarbon on clay minerals, which is of significance for the design of thermal desorption remediation.
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CHEMICAL PHYSICS LETTERS
·
2022
·
IF 2.719
Weiqiu Huang,Bing Zhu,Jiahui Zhu,Xufei Li,Xinya Wang,Baoyou Yan,Fei Yi,Zhen Zhang
Novel AC (termed as A-AC/SiC) with high thermal conductivity was prepared by using emulsified asphalt as precursor and polycarbosilane (PCS) as thermal conductive addition by in-situ reaction. The specific surface area and total pore volume of sample A-AC/SiC-20 was up to 1346 m 2 ·g −1 and 0.89 cm 3 ·g −1 respectively. The SEM and FIIR showed that PCS had been successfully loaded into the A-AC and formed the uniform cross-linking structure, while its thermal conductivity increased by nearly 300 % than that of the parent A-AC. Moreover, it also exhibited high adsorption capacity up to 3.46 mmol·g −1 and excellent recyclability for n-hexane vapor.
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Food Science and Human Wellness
·
2022
·
IF 8.022
Cheng Li,Yang Tian,Jianli Han,Yu Lu,Meiyi Zou,Yue Jia,Chengjian Wang,Linjuan Huang,Zhongfu Wang
β -Conglycinin is one of the major allergens existed in soybean. N -Glycans attached to the β -conglycinin influenced the immunoreactivity and antigen presenting efficiency of β -conglycinin. In this study, we described a new method used to release and collect the N -glycans from β -conglycinin, and the N -glycans existed in linear epitopes of β -conglycinin were identified. Glycopeptides hydrolyzed from β -conglycinin were purified by cotton hydrophilic chromatography. Trifluoromethylsulfonic acid was then used to release glycans from glycopeptides, and new glycopeptides containing one single N -acetyl- D -glucosamine (GlcNAc) moiety were then utilized for mass spectrometry. Five glycosylation sites (Asn-199, Asn-455, Asn-215, Asn-489 and Asn-326) and 22 kinds of glycopeptides were identified. It is noteworthy that the peptide VVN # ATSNL (where # represents for the glycosylation site) was analyzed to be both glycopeptide and linear epitope. Our results provided a new method for the N -glycoform analysis of food allergens, and laid a foundation for understanding the relationship between glycosylation and food allergy.
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JOURNAL OF ELECTRONIC MATERIALS
·
2022
·Vol. 51
·期 12
·6654-6662
·
IF 2.047
Yao Weilin,Cai Chen,Xiang Jiayuan,He Linxuan,Shi Juntao,Chang Xinhao,Ruan Lingfeng,Chen Zihang,Yao Zhujun
The exploration of high-capacity anode materials is extremely vital for the progress of lithium-ion batteries (LIBs). SnSe 2 is of great interest, on account of its low cost and high theoretical specific capacity, when used as the anode of LIBs. SnSe 2 exhibits drastic capacity decay at high rates, due to its inherent low electrical conductivity, as well as its sluggish kinetics and huge volume expansion during charging and discharging. In this work, flexible Sn-based nanofibers were synthesized by electrostatic spinning, followed by high-temperature calcination and selenization to obtain the final SnSe 2 @NCNFs. The SnSe 2 nanoparticles were encapsuled in carbon nanofibers with good ductility after annealing at 600°C. The carbon nanofibers not only act as self-supporting substrates but also improve the conductivity of the composite and retard volume expansion of SnSe 2 . With the above advantages, the integrated SnSe 2 @NCNFs is able to provide good stability, with 144.3 mA h g −1 at 0.5 A g −1 after 1000 cycles. Graphical Abstract
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Xinlei Ding,Yun Chen,Junping Nan,Hengwei Dai,Yuling Wang,Guangmei Bai,Wenge Qiu
N-doped nestlike carbon nanosheets (NCNs-Nx) were prepared successfully by a two-step strategy, namely, the in situ self-assembly hydrothermal synthesis using glucose as the carbon source in the presence of magnesium nitrate and sodium carbonate and the controlled nitrogen doping carbonization using urea as the nitrogen source. The performance of the corresponding Pd/NCNs-Nx catalysts was investigated for the selective hydrogenation of quinolines. The characterization of transmission electron microscopy, nitrogen sorption isotherm measurement, powder X-ray diffraction, X-ray photoelectron spectra, temperature-programmed desorption of pyridine and benzene, and the pyridine adsorption experiments showed that the very high catalytic activities and selectivity of the Pd/NCNs-Nx catalysts were related with the high Pd dispersion and the electronic structure of Pd species as well as the adsorption capacity and the adsorption type of quinoline molecule on the catalyst surface.
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FUEL PROCESSING TECHNOLOGY
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2022
·
IF 8.129
Linlin Liu,Mingwei Zhang,Li Wang,Xiangwen Zhang,Guozhu Li
Bifunctional catalysts with high isomerization activity and mono-branched isomer selectivity are urgently demanded for dewaxing long-chain n -alkanes. In particular, branching location of mono-branched isomer is difficult to control by current techniques. In this study, SSZ-32 zeolite with tunable distribution depth of acid sites in micropore channels is successfully prepared by ion exchange under partial template protection. Loaded with similar Pt nanoparticles , these SSZ-32 catalysts exhibit tunable activity and selectivity for hydroisomerization of n- hexadecane . Characterization results show that the adsorption model and insertion depth of n -alkane is altered by changing the distribution depth of acid sites in SSZ-32 micropore channels. When acid sites distribute in a moderate depth (∼ 4.5 nm) of the micropore channels, high yield of center-position mono-branched isomers (46.85%) is achieved, cracking reaction is significantly inhibited. The mole ratio of 6−/7−/8-methyl isomers to 2−/3-methyl isomers was increased to at least 1.3 times of the traditional catalyst with acid sites distributed throughout the micropores. The cold flow properties of lube base oils in isomerized dewaxing of Fischer-Tropsch wax are improved significantly by achieving an optimal and effective diffusion depth of reaction intermediates in the MTT micropore channels. Efficient and selective hydroisomerization of long-chain n -alkane is realized on Pt/SSZ-32 prepared by the facile partial-detemplation method.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Tiantian Fu,Lingtao Sun,Guijun Li,Yang Xiang,Yibo Tang,Jingqi Sha,Ying Lei,Zhongping Xiong,Yujun Si,Chaozhong Guo
A nitrogen and sulfur codoped carbon-based catalyst (Fe-NS-AG-C) to oxygen reduction reaction (ORR) is prepared by pyrolyzing a precursor from iron chloride, thiourea, anhydrous glucose and carbon black. Glucose is transformed to carbon sheets with defect-rich structures which are highly active to the anchoring of nitrogen and sulfur atoms. Correspondingly, the 3.35 at% and 0.63 at% contents of nitrogen and sulfur in Fe-NS-AG-C are heavily higher than the 0.71 at% and 0.26 at% in the controlled catalyst Fe-NS-C (without glucose). The edge-oriented pyridinic N is easily formed as ORR active sites with the C-S structure. A dual mesopore-dominated microstructure is also constructed by the carbon sheets to favor the mass transfer in the reaction process. As a result, the Fe-NS-AG-C presents outstanding ORR performance with more positive half wave potential, greater limiting current density, and better methanol tolerance than the benchmark Pt/C catalyst. The Zn-air battery assembled with Fe-NS-AG-C outputs 1.48 V of open circuit voltage, 156 mW cm −2 of maximum power density, and 1.26 V of work voltage, 785 mAh g −1 Zn of specific capacity and 983 mWh g −1 Zn of specific energy density at 10 mA cm −2 of discharge current density.
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Nanomaterials
·
2022
·Vol. 12
·期 21
·3870
·
IF 5.719
Shuolin Zhou,Lu Wu,Junzhuo Bai,Min Lei,Min Long,Keying Huang
Levulinic esters, synthesized by the esterification of biomass-derived levulinic acid with various alcohols, is an important chemical that plays an essential role in the fields of biomass fuel additives, organic synthesis, and high value-added products. In the present work, the catalytic esterification of levulinic acid with n-butyl alcohol was selected as a typical model reaction to investigate the catalytic performance of an inexpensive commercial catalyst, titanium oxide nanoparticles. The influences of reaction time, reaction temperature, and catalyst loading on the conversion of levulinic acid to n-butyl levulinate were systematically examined through single-factor experiments. Additionally, the optimization of the reaction conditions was further investigated by a Box–Behnken design in response to the surface methodology. The desired product, n-butyl levulinate, with a good yield (77.6%) was achieved under the optimal conditions (reaction time of 8 h, reaction temperature of 120 °C, and catalyst dosage of 8.6 wt.%) when using titanium oxide nanoparticles as catalysts. Furthermore, it was found that addition of water to the catalytic system facilitated the reaction process, to some extent. This study reveals that the nanosized TiO2material,as an efficient solid acid catalyst, had good catalytic performance and stability for the esterification of levulinic acid after six consecutive uses.Keywords:TiO2nanoparticles;solid acid catalyst;n-butyl levulinate;esterification;response surface methodology
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CRYSTENGCOMM
·
2023
·Vol. 25
·期 11
·1648-1656
·
IF 3.1
Songjie Li,Shilong Su,Yun Tian,Yuanyuan Li,Xiaomei Yu,Panfei Sun,Jin You Zheng
Molybdenum carbide (Mo2C) has become a promising candidate for electrocatalytic hydrogen production from water splitting due to its low price and platinum-like electrocatalytic properties. In this work, Mo2C nanotubes (Mo2C NTs) with ultrathin imbricate structure were successfully synthesized by carburizing polydopamine organic layer covered molybdenum trioxide (MoO3) nanowire templates at elevated temperature through organic–inorganic hybridization. The inner diameter and wall thickness of the as-synthesized Mo2C NTs are about 150 nm and 100 nm, respectively. Two-dimensional Mo2C nanoflakes with a thickness of about 10 nm were composed of nanoclusters with a size of 2 nm. Furthermore, N–MoxC was facilely prepared by nitrogen doping into the prepared Mo2C by chemical vapor deposition and the enhanced electrocatalytic activity was obtained with an overpotential of 120 mV at a current density of 10 mA cm−2. An enlarged specific surface area of 189 m2 g−1 was achieved for N–MoxC, which provides more electrocatalytic active sites for water reduction. More importantly, the interface optimization of Mo2C and MoC was expected to modify the electronic structure and accelerate the electron transfer for improved water splitting performance.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2023
·
IF 4.4
Shangjun Lin,Wentao Liu,Xuehe Hou,Zhenyun Peng,Zhencheng Chen,Fangrong Hu
As an organic substance, n -propanol gas has been paid attention to in environmental monitoring and exhalation of lung cancer patient. In this paper a rapid detection method for n -propanol gas is developed based on molecularly imprinted polymers (MIP) and terahertz (THz) metasurface sensors. We first prepared a MIP suitable for detecting the n -propanol gas. And then the n -propanol MIP was modified to the THz metasurface sensor for detecting the n -propanol gas. Since the MIP adsorbed with n -propanol changes the dielectric environment of the sensor, the resonance frequency of the sensor also change. So we based on the n -propanol concentration was analyzed according to the change in resonance frequency. The experimental results showed that the sensor can effectively detect the n -propanol concentration in the range of 50–500 ppm (parts per million). In addition, we also verified the specificity and repeatability of the sensor. This work provides a new idea and method for the sensitive and specific detection of n -propanol gas.
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AICHE JOURNAL
·
2022
·Vol. 68
·期 7
·e17677
·
IF 4.167
Shen Hu,Jiaxuan Chen,Qunfeng Zhang,Junru Liu,Jinlin Meng,Guanghua Ye,Xinggui Zhou,Weikang Yuan
Surface barriers persist in the molecular transport across external crystal surface of zeolites, which brings strong influences on zeolite catalysis. This study probes the role of crystal-size–dependent surface barriers in zeolite catalysis, with n -pentane isomerization catalyzed by Pt/ZSM-5 as a model reaction system. Chemical liquid deposition of SiO 2 is performed to reduce surface barriers on ZSM-5 crystals with different sizes. After SiO 2 deposition, surface barriers on both small (266 nm) and large (1304 nm) crystals are significantly reduced, while the improvement in catalytic activity for the large crystals (76.1%–129.1%) is much higher than that for the small ones (−17.4% to 16.7%). For the large ZSM-5 crystals, diffusion limitation is stronger, and thus the effect of surface barriers on catalytic activity is more important. This study reveals the unique role of crystal-size–dependent surface barriers in zeolite catalysis, and understanding this is important for the optimal design of zeolite catalysts.
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