NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 47
·期 3
·1308-1317
·
IF 3.925
Xuebin Hou,Zelong Huang,Liu Hu,Qufu Wei,Yi Hu
Construction of molybdenum phosphides (MoP) that are connected to conductive composite materials has been demonstrated to be an effective strategy for improving the activity of MoP, and it is crucial for both the hydrogen evolution reaction (HER) and lithium-ion batteries (LIBs). However, increasing the exposed active sites and simultaneously enhancing the synergistic effect between MoP and the conductive substrate is challenging. Herein, constructing a multi-hierarchical conducting connection based on carbon nanoparticles and reduced graphene oxide (rGO) sheets was proposed. MoP nanoparticles were in situ grown in a carbon matrix to form flower-like MoP/C particles and were well scattered in stable lamellar rGO nanosheets. Benefiting from the conductive network and good dispersion of active sites, the resultant MoP/C-rGO hybrid exhibits efficient HER activity, with Tafel slopes of 69 mV dec−1 and 87 mV dec−1 under acidic and alkaline conditions. Significantly, even when applied as an anode for LIBs, it demonstrates excellent storage performance with a high specific capacity and long-term stability. It displays superior cycle performance of a reversible capacity of 624.6 mA h g−1 at 0.5 A g−1 after 500 cycles. This work provides insight into the construction of multi-hierarchical structures for efficient bifunctional nanostructural electrodes for energy conversion and storage.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yaqi Xue,Haihong Xia,Jing Li,Jiantao Su,Fei Ge,Xiaohui Yang,Jianchun Jiang,Minghao Zhou
Catalytic transfer hydrogenation (CTH) was recognized as a promising technique for converting various lignin derivatives to fuels and high-value compounds in heterogeneous systems. Herein, Co@C catalysts with diverse organic ligands, Keggin-type heteropolyacids, acid addition quantities, and metal/organic ligand molar ratios were synthesized via one-pot hydrothermal processes and carbonization methods. The optimized catalyst demonstrated highly efficient active hydrogen generation from isopropanol and the best conversion (100 %) for vanillin (VAN) hydrodeoxygenation (HDO) with 90 % 2-methoxy-4-methylphenol (MMP) yield at 180 °C for one hour under mild conditions of 0 MPa N 2 (hydrogen-free circumstance), which were strongly connected to the higher specific surface area (154.45 m 2 /g), acidic site density (4.67 mmol/g), and stronger metal-P interactions of the Co(H 4 )@C-HPW 0.25 catalyst. The findings in this work provided an advanced thinking for designing high-performance non-noble-metal catalysts that could be applied in the catalytic HDO transformation of various biomass derivatives into green fuel and chemicals under mild circumstances.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Guolong Lu,Xin Men,Ruoqi Tang,Zhida Wang,Hao Cui,Tongxi Zheng,Mi Wang,Haoqi Yang,Zhenning Liu
Transition metal and nitrogen co-doped carbon electrocatalysts are promising candidates to replace the precious metal platinum (Pt) in oxygen reduction reactions (ORR). Unfortunately, the electrochemical performance of existing electrocatalysts is restricted due to limited accessibility of active sites. Inspired by jellyfish tentacles, we design an efficient ORR micro-reactor called Fe-N x /HC@NWs. It features abundant exposed Fe-N x active sites dispersed on nitrogen-doped cubic carbon cages, which have a hierarchically porous and hairy structure. The accessible, atomically dispersed Fe-N x sites and the elaborate substrate architecture synergize to provide the catalyst withremarkable ORR catalytic activity, extraordinary long-term stability, and favorable methanol tolerance in an alkaline electrolyte ; overall, its performance is comparable to that of commercial carbon-supported Pt. Our synthesis is facile and controllable, paving a new avenue toward advanced non-precious metal-based electrocatalysts for energy storage and conversion .
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Bingyang Liu,Yu Wang,Xue Hao,Xuetao Liang,Qi Yang
In this work, a carbon-based catalyst Fe/Co@C with MOF as a self-sacrificing template was prepared by high-temperature roasting of FeCo-MIL101, which was applied to activate PMS for the degradation of chlorotriazine herbicides (ATZ and SIM) showing excellent performance. Characterization analysis revealed that Fe/Co@C possesses a certain graphene structure and has a saturation magnetization rate of 0.87 emu/g, which can be separated from the solution easily and quickly. The degradation of ATZ and SIM was enhanced by introducing chloride ions into the system, and 100 mmol/L Cl - could lead to the complete removal of ATZ and SIM in 6 min, while improving the interfacial electron transfer of Fe/Co@C/PMS. In combination with quenching experiments, ESR test results and DFT calculations, two important roles of chlorine radicals in the reaction are proposed: (1) direct electron transfer and (2) indirect promotion of 1 O 2 generation through the production of HOCl. In addition, the testing of the influencing factors of the catalyst in the system (catalyst dosing, PMS dosing, pH, temperature), the testing of coexisting anions in the aqueous matrix, and the reusability all showed satisfactory performance. Finally, the degradation mechanisms of ATZ and SIM were proposed in combination with GC–MS determination of contaminant intermediates and analysis of their toxicity.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Xuanning Qin,Han pang,Zebin Yu,Zuoyu Qin,Ronghua Jiang,Shuangquan Yao,Jun Huang,Yanping Hou,Ben Fan
Accelerating electron transfer and exposing active sites are key factors that could improve electrocatalytic hydrogen evolution reaction (HER). In this study, Co 3 S 4 -Ni 3 S 2 -C/N, the cactus bulb-shaped nanoparticles based on metal-organic frameworks (MOFs), were successfully prepared. The catalyst requires only 101 and 227 mV overpotential to reach current densities of 20 and 100 mA cm −2 , respectively, in 1 M KOH. The high catalytic activity is attributed to the confinement effect achieved by introducing 2-aminoterephthalic acid as a precursor, allowing the catalyst to have a small particle size and fully exposed metal active sites. Moreover, the catalyst has a highly conductive metal-S-C/N channel that effectively reduces the intrinsic charge transfer resistance of the catalytic electrode, improves its conductivity, and modulates the electron density at the metal active site. Furthermore, compared to other crystal planes, the exposed (111) crystal plane of Co 3 S 4 provides the most octahedral coordination of high spin state Co 3+ , which is highly catalytically active. This makes it the dominant crystal plane for catalysis. Through spatial confinement effect to limit metal sulfide particle size and introducing an organic backbone to create highly conductive metal-S-C/N channels, our study provides a general approach to developing highly active catalytic materials.
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JOURNAL OF ASIA-PACIFIC ENTOMOLOGY
·
2023
·
IF 1.5
Shanshan Gao,Xinyi Zhang,Can Zhou,Guangyan Zhang,Yonglei Zhang,Ruimin Li,Kunpeng Zhang
Insect odorant binding proteins (OBPs) paly an important role in the recognition and transmission signals. One odorant binding protein gene, TcasOBP7G , was significantly up-regulated after exposure to eucalyptol. Nevertheless, the causal role of TcasOBP7G in Tribolium castaneum is still unclear. Here, TcasOBP7G was cloned and characterized from T. castaneum , aligning with the typical characteristic of Minus-C OBPs. The analysis of gene expression profile showed that TcasOBP7G is highly expressed at late larval and adult stage, with particularly high expression levels in ovary and testis of adults, suggesting that TcasOBP7G might be associated with reproduction of T. castaneum. Furthermore, RNAi of TcasOBP7G led to a decrease in spawning, while the development of gonads was normal, suggesting that TcasOBP7G may medicate the reproduction of T. castaneum . Additionally, the mRNA level of TcasOBP7G was significantly increased after exposure to eucalyptol, and knockdown of TcasOBP7G resulted in an increased susceptibility of T. castaneum to eucalyptol, indicating that TcasOBP7G is associated with the tolerance of T. castaneum to eucalyptol. Altogether, these results indicate that TcasOBP7G is required for both reproduction and defense against phytochemical in T. castaneum . This study will provide a theoretical basis for the development of novel control strategies based on the olfaction of insects.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
·
2023
·
IF 4
Zong-Bao Yu,Zhuozhuo Song,Peng Zheng,Jie Sun,Zhanxu Yang
Transition metal sulfides (TM sulfides) has long been regarded as highly promising materials for catalyzing oxygen evolution reaction (OER). The function of TM sulfides in OER occurs on TM oxyhydroxide and SO 4 2− , which are formed through surface reconstruction under certain potentials. It is worth noting that the impact of SO 4 2− on the local charge distribution among atoms, a crucial determinant of OER performance, has been insufficiently studied. This study aims to investigate the role of SO 4 2− in mediating the partial redistribution of charges among Co, Ni and O atoms on a precatalyst Co 9 S 8 /C–Ni(OH) 2 electrode. The electrode undergoes self-reconstruction to form a CoOOH/SO 4 2− /NiOOH structure on its surface that is active for the OER. The results demonstrate that SO 4 2− facilitates the local charge redistribution of active atoms, leading to optimized adsorption energy of OER intermediates and increased redox center of the material. Furthermore, SO 4 2− serves as an electron mediator in the OER process under varying applied voltages. Consequently, CoOOH/SO 4 2− /NiOOH achieves a Tafel slope of 56 mV dec −1 , an overpotential of 250 mV, and maintains a high stability for over 100 h at a current density of 20 mA cm −2 . Overall, this research provides valuable insights into catalytic reaction mechanisms and the design of efficient composite catalysts.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Ying Liao,Yue Pan,Xiang Feng,Xiaobo Chen,Yibin Liu,Chaohe Yang,Hao Yan
Designing efficient active sites to facilitate the oxidation of hydroxyl group to carboxylic acid under the influence of nitrogen-containing functional groups is worth exploring, but it is rarely investigated. Herein, we construct defective Au-ZrO 2 interfacial structures by tuning the calcination temperature of ZrO 2 support to boost the oxidation of amino alcohols to amino acids. Interestingly, the modification of calcination temperature induces the escape of saturated coordination oxygen atoms in ZrO 2 support, leaving behind abundant surface oxygen vacancy (O v ). The as-formed Au δ− -O v interfacial site displays the unique synergistic adsorption effect and electron transfer ability. Specifically, the O v site voluntarily adsorbs the –NH 2 group of amino alcohol, thus ensuring that the electron-rich Au δ− nearby O v site adsorbs the hydroxyl groups and activates the C-H bond activation of NH 2 CH 2 CH 2 O* intermediates. Consequently, Au/ZrO 2 -600 catalyst with more defective Au δ− -O v interfacial sites exhibits 98.8 % product yield for the oxidation of diethanolamine to iminodiacetic acid at only 30 °C. The catalyst system is further extended to the oxidation of other amino alcohols, involving monoethanolamine and triethanolamine, to their corresponding amino acids with excellent catalytic performance.
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POLYMER COMPOSITES
·
2021
·Vol. 42
·期 6
·3000-3010
·
IF 3.171
Peng Yin,Zhicheng Shi,Liang Sun,Peitao Xie,Davoud Dastan,Kai Sun,Runhua Fan
Polymer nanocomposites with high energy-storage capability have been widely used in electronic devices. To achieve further enhanced energy density, developing nanofillers with tailored compositions and nanostructures is demonstrated to be an effective strategy. Especially, hybrid nanoparticles (NPs) with abundant internal interfaces are acknowledged as a promising candidate. Here, a class of carbon/silica hybrid nanoparticles (C/SiO 2 h-NPs) with disorderly mixed nanostructures are synthesized and employed to prepare C/SiO 2 h-NPs/polyimide nanocomposites. To reveal the influence of internal interfaces on dielectric properties, a series of comparative composites co-filled with C and SiO 2 NPs are also prepared. The breakdown strength of the C/SiO 2 h-NPs/polyimide composites can reach 303.96 kV/mm, which is over 200% that of their counterparts. It is believed that the abundant heterogeneous interfaces inside the C/SiO 2 h-NPs can effectively impede the development of conductive paths, thereby obviously enhancing breakdown strengths. Furthermore, the C/SiO 2 h-NPs/polyimide composite with 5 wt% C/SiO 2 h-NPs demonstrates a high discharged energy density of ~0.612 J/cm 3 at 150 kV/mm, which is about 2.29 times higher than pure polyimide (PI) (~0.267 @ 150 kV/mm), along with a high discharge energy efficiency of 85.9%. This work offers a practicable strategy for the design of functional NPs toward high-performance dielectric composites.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Li Gong,Xiaojiang Qiu,Paul G. Tratnyek,Chengshuai Liu,Feng He
FeNX in Fe single-atom catalysts can be the active site for adsorption and activation of reactants. In addition, FeNX species have been shown to facilitate electron transfer between Fe and the carbon supports used in newly developed metal–air batteries. We hypothesized that the combination of FeNX species with granular zero-valent iron (ZVI) might result in catalyzed reductive decontamination of groundwater contaminants such as trichloroethylene (TCE). Here, such materials synthesized by ball milling microscale ZVI with melamine and the resulting N species were mainly in the form of pyridinic, pyrrolic, and graphitic N. This new material (abbreviated as N–C-mZVIbm) dechlorinated TCE at higher rates than bare mZVIbm (about 3.5-fold) due to facilitated electron transfer through (or around) the surface layer of iron oxides by the newly formed Fe–NX(C). N–C-mZVIbm gave higher kTCE (0.4–1.14 day–1) than mZVIbm (0–0.4 day–1) over a wide range of pH values (4–11). Unlike most ZVI systems, kTCE for N–C-mZVIbm increased with increasing pH values. This is because the oxide layer that passivates Fe0 at a high pH is disrupted by Fe–NX(C) formed on N–C-mZVIbm, thereby allowing TCE dechlorination and HER under basic conditions. Serial respike experiments gave no evidence of decreased performance of N–C-mZVIbm, showing that the advantages of this material might remain under field applications.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 18
·8045-8053
·
IF 3.591
Yaping Zhang,Daofei Lv,Jiayu Chen,Zewei Liu,Chongxiong Duan,Xin Chen,Wenbing Yuan,Hongxia Xi,Qibin Xia
The separation of ethylene/ethane mixtures using energy-efficient technologies is important but challenging. In this study, we prepared a Zr-based metal–organic framework (MOF-545) possessing a high Brunauer–Emmett–Teller (BET) surface area of 2265.4 m2 g−1, and investigated its adsorption performance for ethylene/ethane separation. Isotherm measurements show that MOF-545 exhibits preferential adsorption of ethane over ethylene. The mechanism underlying the selective adsorption of ethane over ethylene was revealed by the calculations of preferential adsorption sites, interaction energies and adsorption density distributions of ethane and ethylene in MOF-545 via the Metropolis Monte Carlo method. Results show that the strong C–H⋯N hydrogen bonding between ethane molecules and porphyrin rings gives rise to the selective adsorption of ethane over ethylene. Thermal, air and cycling stability tests, adsorption selectivity and adsorption enthalpy calculations, and breakthrough experiments comprehensively validate the potential of MOF-545 as an efficient ethane-selective adsorbent for ethane/ethylene separation.
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ENVIRONMENTAL MICROBIOLOGY
·
2021
·Vol. 23
·期 6
·3265-3273
·
IF 5.491
Mingliang Zhang,Yijun Ren,Shilong Du,Yidong Zhou,Wankui Jiang,Zhijian Ke,Mingli Jiang,Jiguo Qiu,Jian He,Qing Hong
Summary Pymetrozine is a synthetic pesticide that can be utilized as the sole carbon source by Pseudomonas sp. strain BYT-1. However, the genes involved in the degradation of pymetrozine remain unknown. We used transposon mutagenesis to create a mutant that unable to hydrolyze pymetrozine. The transposon interrupted the gene pyzH , which was cloned by self-formed adaptor PCR. PyzH hydrolyzed the C=N double bond of pymetrozine to produce 4-amino-6-methyl-4,5-dihydro-2 H -[1,2,4]triazin-3-one (AMDT) and nicotinaldehyde; the latter inhibits PyzH activity. PyzH can completely hydrolyze pymetrozine in the presence of dehydrogenase ORF6, which can convert nicotinaldehyde into nicotinic acid and relieve the inhibition. H 2 18 O-labeling experiments showed that the oxygen atom of nicotinaldehyde came from water instead of oxygen. PyzH homologous genes were also found in other soil isolates able to degrade pymetrozine.
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