FUEL PROCESSING TECHNOLOGY
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2023
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IF 7.5
Mengjiao Fan,Yuewen Shao,Kai Sun,Yuchen Jiang,Shu Zhang,Yi Wang,Song Hu,Jun Xiang,Xun Hu
Bio-oil as a carbon source can be used to prepare hybrid metal@carbon material while the polymerization of which generally prevents metals from exposure. In this study, melamine was used as a structural regulating agent for preparing Co/N/C catalyst via heating the mixture of cobalt nitrate, melamine and bio-oil for hydrogenation of o-chloronitrobenzene (o-CNB). The results showed that the Co species was encapsulated in the carbon structure from cross-polymerization of melamine and bio-oil at 600 °C. The further heating to 900 °C led to decomposition of melamine-derived substance, and meanwhile cobalt oxide was reduced and confined in the resulting carbon structure. The formed metallic Co catalyzed the growth of long carbon nanotube with cobalt on the tip, forming the Co/N/C catalyst of higher specific surface area (128.2 m 2 /g) and metallic Co dispersion (3.7%), rendering the superior activity for hydrogenation of o-CNB with the yield of o-chloroaniline up to 90.2%. The encapsulation or exposure of Co species was closely related to relative ratio of bio-oil and melamine in the catalyst precursors. Additionally, leaching of cobalt, due to dechlorination of o-CNB, was found to be an issue of Co/N/C catalyst but not for that of Ni/N/C catalyst.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Lu Tian,Dazhong Zhong,Tao Zhao,Yi Liu,Lu Hao,Qiang Fang,Xuelei Lang,Xin Zhao,Genyan Hao,Guang Liu,Jinping Li,Qiang Zhao
Developing highly efficient OER catalysts is essential for producing hydrogen from water electrolysis to compensate for conventional fossil fuel shortages. Here, the oxygen-vacancy-rich heterostructure grown on the Ni foam (NF) (Co 3 O 4 @Fe-B-O/NF) is fabricated. The synergistic effect between Co 3 O 4 and Fe-B-O has been proven effectively modulate the electronic structure and produce highly active interface sites, ultimately leading to enhanced electrocatalytic activity. Co 3 O 4 @Fe-B-O/NF requires an overpotential of 237 mV to drive 20 mA cm −2 in 1 M KOH, and 384 mV to drive 10 mA cm −2 in 0.1 M PBS, superior to most catalysts currently used. Moreover, Co 3 O 4 @Fe-B-O/NF as an oxygen evolution reaction (OER) electrode shows great potential in overall water splitting and CO 2 reduction reaction (CO 2 RR). This work may provide effective ideas for designing efficient oxide catalysts.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2023
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IF 6.1
Zhengming Xu,Shuang Liu,Huining Lai,Lijun You,Zhengang Zhao
Arbutin, salidroside, polydatin, and phlorizin are typically natural bioactive phenolic glycosides. To improve the liposolubility and bioavailability, highly liposoluble derivatives including 6′-O-lauryl arbutin, 6′-O-lauryl salidroside, 6″-O-lauryl polydatin, and 6″-O-lauryl phlorizin were efficiently synthesized by enzymatic acylation in a green solvent 2-MeTHF. Their reaction conversions reached 84.4, 99.5, 99.8, and 89.1%, respectively, when catalyzed by Lipozyme 435 at 20 mg/mL at 50 °C. As expected, the derivatives had high log P (1.66–2.37) and retained good antioxidant activity, making them potential alternatives to butylated hydroxytoluene (BHT) and tert-butyl-hydroquinone (TBHQ) in lipid systems. Then, the intestinal permeability characteristics and metabolism of phenolic glycosides and their derivatives were investigated based on Caco-2 monolayers. The permeability of polydatin and phlorizin was mainly through active transport, but that of arbutin and salidroside involved both passive diffusion and active uptake. The acylated derivatives suffered from severe CES-mediated hydrolysis but exhibited a larger transported amount than phenolic glycosides.
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Materials
·
2022
·Vol. 15
·期 24
·8811
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IF 3.748
Wei Wang,Le Pang,Ming Jiang,Yaping Zhu,Fan Wang,Jingwen Sun,Huimin Qi
Silicon-based ceramic aerogels obtained by the polymer pyrolysis route possess excellent thermophysical properties, but their poor mechanical properties limit their broader applicability in thermal insulation materials. Herein, SiCN(O) ceramic aerogels were prepared under the toughening effect of a crosslinker (hexamethylene diisocyanate, HDI), which maintains the structural integrity of the aerogel during the wet gel-to-aerogel conversion. The aerogel maintained a high surface area (88.6 m2g−1) and large pore volume (0.21 cm3g−1) after pyrolysis. Based on this, mullite-fiber-reinforced SiCN(O) aerogels composites with outstanding thermal insulation properties and better mechanical performance were synthesized via ambient pressure impregnation. Furthermore, the effect of the impregnation concentration on the mechanical and insulation properties of the composites was investigated. The results revealed that the composite prepared with a solution ratio of 95 wt.% exhibited a low density (0.11 g cm−3) and a low thermal conductivity (0.035 W m−1K−1), indicating an ~30% enhancement in its thermal insulation performance compared to the mullite fiber; the mesoporous aerogel structures wrapped on the mullite fibers inhibited the gas thermal conduction inside the composites.Keywords:SiCN(O) ceramic aerogel;composite;pore structure;thermal conductivity;ambient pressure impregnation;thermal insulation optimization
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FUEL
·
2022
·
IF 8.035
Zejun Zhang,Zhansheng Wang,Qingji Wang,Hua Zhang,Yuqi Tang,Qian Qu,Liwei Shen,Dong Xiang,Yuanzhu Mi,Xuemin Yan
A multi-branched trinuclear ionic liquid demulsifier (EDHBr-IL) was synthesized using glycerol triglycidyl ether, di- n -hexylamine and 1-bromododecane as raw materials using a simple “one-pot” method. Its structure was characterized by FT-IR, 1 H NMR and 13 C NMR spectra. EDHBr-IL exhibited a favorable demulsifying performance in W/O emulsions at lower temperature. The demulsifying efficiency (DE) of 300 mg/L of EDHBr-IL at 50 °C reached 90 % with for 2 h. It showed an excellent acid, alkaline and salt resistance. A relatively high DE was achieved at a pH range of 4–12 and a salinity of 10,000 mg/L. In addition, the demulsification mechanism was explored based on interfacial properties and micro examination. EDHBr-IL has substantial potential for the demulsification of W/O emulsions due to its simple and safe preparation, and performance comparable to that of with commercial demulsifiers.
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Zhen Pu,Jianwei Qin,Xiaoguo Fu,Ruizhi Qiu,Bin Su,Maobing Shuai,Fang Li
Fundamental investigation of metal–CO interactions is of great importance for the development of high-performance catalysts to CO activation. Herein, a series of side-on bonded mononuclear lanthanide (Ln) oxocarbonyl complexes OLn(η2-CO) (Ln = La, Ce, Pr, and Nd) have been prepared and identified in solid argon matrices. The complexes exhibit uncommonly low C–O stretching bands near 1630 cm–1, indicating remarkable C–O bond activation in these Ln analogues. The η2-CO ligand in OLn(η2-CO) can be claimed as an anion on the basis of the experimental observations and quantum chemistry investigations, although the CO anion is commonly considered to be unstable with electron auto-detachment. The CO activation in OLn(η2-CO) is attributed to the photoinduced intramolecular charge transfer from LnO to CO rather than the generally accepted metal → CO π back-donation, which conforms to the traditional Dewar–Chatt–Duncanson motif. Energy decomposition analysis combined with natural orbitals for chemical valence calculations demonstrates that the bonding between LnO and η2-CO arises from the combination of dominant ionic forces (>76%) and normal Lewis “acid–base” interactions. The fundamental findings provide guidelines for the catalyst design of CO activation.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Guang-Rong Ding,Yao-Feng Wang,Guo-Yi Duan,You-Qian Fan,Bao-Hua Xu
In this study, a tungstated zirconia (WOx/ZrO2) catalyst was developed for the continuous synthesis of adiponitrile (ADN) by gas-phase nitrilation of dimethyl adipate (DMA) with NH3. The highest TOFADN could be reached on WOx/ZrO2 bearing ∼1D WOx species (highly dispersed and discontinuous status) at the surface, which, however, delivered the poorest selectivity toward nitrilation (SADN+MCP). In comparison, both efficient and selective transformation of DMA to ADN was achieved by fabricating WOx/ZrO2 with continuously distributed oligomeric WOx species (∼2D) at the surface, either by varying the dosage of the W-reagent in the preparation of WOx(m)/ZrO2 or by doping a proper amount of the Mn element into WOx(5.0)/ZrO2, bearing WO3 NPs. Furthermore, the in situ diffuse reflectance infrared Fourier transform spectroscopy investigations of both independent and competitive adsorptions of ester functionality and NH3 over W–O–Zr, W–O–W, and Zr–O–Zr boundaries at the surface clarified the synergistic effect of these species in the activation of DMA/NH3 and thereby nitrilation.
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Molecular Catalysis
·
2023
·
IF 4.6
Zong-Pin Fu,Yun-Peng Zhao,Fa-Peng Wu,Jin-Xuan Xie,Le-Le Qiu,Jian Xiao,Jing Liang,Yong-Hui Bai,Fang-Jing Liu,Jing-Pei Cao
The selective hydrogenolysis of C O bonds is critical for the effective valorization of lignin. Herein, we synthesized a series of highly efficient Ni x Co y Al-T catalysts by a coprecipitation-calcination-reduction method and evaluated their catalytic hydrogenolysis performance towards the C O bonds of lignin-derived aryl ether, using isopropanol as the hydrogen donor source. The results revealed that the Ni 0.5 Co 1.5 Al-600 catalyst displayed superior activity and its catalytic performances were strongly influenced by the Ni/Co molar ratios and calcination temperatures. The enhanced dispersion of metal particles and the electron transfer from Ni to Co in Ni 0.5 Co 1.5 Al-600 catalyst facilitated the cleavage of C O bonds in lignin model compounds. Furthermore, the β-benzyl-H atom in 2-phenoxy-1-phenylethanol (PPE) also contributes to the cleavage of C aliphatic -O bonds. Under optimized reaction conditions (180 ℃, reaction time 2 h), PPE was completely converted over the Ni 0.5 Co 1.5 Al-600 catalyst, and the yield of ethylbenzene and cyclohexanol reached 95.91wt% and 85.73wt%, respectively. These findings demonstrate that the Ni x Co y Al-T catalytic system holds great promise for the production of valuable chemicals from lignin under mild conditions.
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BIOMATERIALS
·
2023
·
IF 14
Zheng Zou,Zhen Zhang,Hui Ren,Xueliang Cheng,Xuesi Chen,Chaoliang He
Injectable antibacterial hydrogels have attracted considerable attention in wound management. However, the development of injectable hydrogels with excellent antibacterial activity , good biocompatibility , and strong tissue adhesion remains a challenge. In this study, an antibacterial tissue-adhesive hydrogel was developed based on a catalyst-free o -phthalaldehyde (OPA)/amine reaction by simply mixing OPA-terminated four-arm poly(ethylene glycol) (4aPEG-OPA) and ε-poly- l -lysine (ε-PLL) solutions. The hydrogel showed tunable gelation time, storage moduli , and degradation rate depending on the polymer concentration and 4aPEG-OPA/ε-PLL mass ratio. The hydrogel exhibited nearly 100% bacterial inhibition rates in-vitro against Gram-negative E. coli and Gram-positive S. aureus , while maintaining good biocompatibility. The hydrogel matched well in shape and tightly adhered to the tissue after in-situ formation at the wound sites. Following the treatment of rat models of full-thickness skin incisions and round wounds, the hydrogel effectively closed the wounds and promoted wound healing. Moreover, after administering to S. aureus infected full-thickness skin wounds, the hydrogel exhibited remarkable efficacy in inhibiting wound infection with a bacterial inhibition rate over 99.94%, achieving a significantly accelerated wound healing compared with the commercially available Prontosan® gel. Therefore, the hydrogel exhibits great potential as a wound dressing for infection prevention and promotion of healing.
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TOXICOLOGY AND APPLIED PHARMACOLOGY
·
2022
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IF 4.46
Wen Chen,Pengcheng Tu,Xiang Ye,Qiong Tang,Ting Yu,Xiaodong Zheng
Microplastic particles degraded from plastic litters are recognized as a global environmental pollutant, which can be transferred and enriched via the food chain to impact ecosystems and human health. A balanced gut microbiota contributes to human health through host–gut interactions, environmentally-driven factors such as microplastic exposure would disturb the gut bacteria and affect its functionality. Dietary compounds can remodel the compositions of gut microbes, and interact with bacteria exerting profound effects on host physiology. This study explored the effects of bayberry-derived anthocyanin cyanidin-3-O-glucoside (C3G) and microplastic polystyrene (PS) on the gut microbiome in C57BL/6 mice, especially the alterations in gut bacteria and its metabolites. Using 16S rRNA high-throughput sequencing, variations in gut bacterial composition and enrichment of functional pathways were found upon PS and C3G administration. Meanwhile, the differential metabolites and metabolic pathways were identified by metabolomic analysis. Importantly, colonic and fecal PS levels were found to be strongly correlated with key microbiota-derived metabolites, which are associated with xenobiotic metabolism via regulation of xenobiotics-metabolizing enzymes and transporters. These results may offer new insights regarding the protective effects of C3G against xenobiotic PS exposure and the roles of gut bacterial metabolites.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
·
2022
·
IF 4.383
Baogang Su,Hui Pan,Linbo Li,Linjun Shao,Chenze Qi,Shujing Zhou,Jinjing Li
Design and preparation of highly active and stable supported palladium catalysts have garnered increased attention for their easy separation and reusability. Herein, MCM-41 mesoporous materials functionalized by four different amino functional groups were synthesized by using four commercially available siloxanes and then used to support palladium catalysts. The Fourier transform infrared spectroscopy (FT-IR) was used to analyze the chemical structures of functionalized MCM-41 supports. The thermogravimetric analysis (TGA) and element analysis (EA) were employed to determine the grafting densities of functional groups on MCM-41 supports. The mesoporous structures of functionalized MCM-41 supports and dispersion of palladium species were characterized by high resolution transmission electron microscopy (TEM) and X-ray diffraction patterns (XRD). A study of the materials using positron annihilation lifetime spectroscopy (PALS) reveals the different ortho-positronium ( o -Ps) annihilation properties of the supported palladium species on the four supports. Meanwhile, the catalytic activities of supported palladium species on the four supports were evaluated by the Heck reactions of iodobenzene with n-butyl acrylate. At last, the annihilation properties of the supported palladium species on the four supports were successfully correlated with their catalytic activities. The result suggests a facile method to determine and predict the catalytic activities of supported palladium species by using PALS, which may hold great potential in the preparation of rationally designed and highly active supported palladium catalysts.
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Materials Today Chemistry
·
2022
·
IF 7.613
Z. Cheng,H. Yang,Y. Xu,J. Jiang,Q. Xu
Fabrication of active and durable non-noble metal heterogeneous electrocatalysts to settle the relatively slow kinetic process and poor stability during the oxygen evolution reaction (OER) process is of great significance. Herein, we fabricate in-situ 2D Fe-based trimetallic complex spinel oxide nanosheets (FeCoNi)O 4 via a polyethylene glycol-barbituric acid deep eutectic solvent-assisted route. Multiple analytical characterizations illustrate a deep understanding of the structure and composition of (FeCoNi)O 4 , disclosing Fe, Co, and Ni ions occupy both tetrahedrally and octahedrally coordinated positions. Meanwhile, the synergistic actions of preparing multiple-cations substitution and constructing oxygen vacancy activate covalent Fe–O–Co bonds in (FeCoNi)O 4 . Due to the active bimetallic Fe–O–Co sites, enhanced electronic conductivity and unique structure stability, the synthesized 2D (FeCoNi)O 4 nanosheets exhibit excellent OER performance with relatively low overpotential (421 mV for 1000 mA/cm 2 ) and long-term stability (720 mA/cm 2 for 6 h) in alkaline media, which is much better than that of Fe-based bi/monometallic spinel oxides. In-situ Raman spectra and quasi-in-situ X-ray photoelectron spectroscopy results depict that O-bridged Fe–O–Co bimetallic sites promote the formation of μ(O–O) intermediates and undergo the direct O 2 evolution route, thus accelerating OER.
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