CRYSTENGCOMM
·
2024
·
IF 2.6
Guixin Zhao,Sixuan Zhang,Jinzhao Huang,Zehui Liu,Feng Jiao,Ke Zhang,Yu Zhang,Xiaolong Deng
NiMo-based polyalloy catalyst is a non-precious metal-based high-entropy alloy catalyst that has been extensively studied in recent years. It exhibits superior electrochemical performance in electrocatalytic water splitting for hydrogen production, and the combination of NiMo-based polyalloy catalysts with carbon black substrates is expected to produce better electrochemical supports. In this paper, we prepared a series of carbon-based high-entropy heterogeneous material catalysts using zero-dimensional carbon black, one-dimensional carbon nanotubes and two-dimensional graphene as substrates, respectively. Analytical results through structural characterization of the synthesized materials as well as electrochemical tests revealed that carbon black, which is in the form of nanoparticles, can be more tightly wrapped with Ni shells compared to tubular nanotubes and flake graphene, which can effectively increase the number of active sites, thus promoting the outstanding performance of the zero-dimensional carbon-based transition metal nanomaterial catalysts NiMoCoMnLa/CB@Ni in alkaline electrocatalytic hydrogen precipitation reaction . Driven by these findings, this work may provide new ideas in the pathway of rationally designing zero-dimensional carbon-based high-entropy alloy nanoparticle catalysts as efficient electrocatalysts in green hydrogen production processes.
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高影响因子
FUEL
·
2025
·
IF 7.5
Hong-Hui Gong,Xian-Yong Wei,Wen-Long Mo,Zhi-Min Zong,Guang-Hui Liu,Pei Liu,Kun-Peng Jiao
NiCs/Al 2 O 3 with medium-strong alkaline and the contents of Ni and Cs of 26.55 wt% and 0.02 wt%, respectively, was prepared by a three-step method and characterized with multiple tools. Oxydibenzene (ODB) and benzyloxybenzene (BOB) were used as low-rank coal-related model compounds and their catalytic hydroconversion (CHC) were investigated over NiCs/Al 2 O 3. Under mild conditions (MCs), NiCs/Al 2 O 3 can effectively activate H 2 to biatomic active hydrogen (H···H) and part of H···H can be effectively split to relative mobile H - and immobile H + on the NiCs/Al 2 O 3 surface. Both ODB and BOB can be completely converted and full hydrogenation (FH) of the benzene ring (BR) in −O-BR is the first step for the CHC of both ODB and BOB via H···H transfer to the BR under MCs. Subsequently, H - transfer to an ipso -carbon (IC) in the resulting oxydicyclohexane from the FH of ODB cleaves an −O-CH< bond to produce cyclohexane (CH I ) and cyclohexyloxy anion (CHOA), which abstracts H + from H···H to afford cyclohexanol (CH II ) followed by H - transfer to the IC in CH II and subsequent HO – release to yield CH I . As a result, CH I is the only final product from the CHC of ODB. In contrast, H - transfer preferentially proceeds to the carbon atom in the –CH 2 - of the resulting benzyloxycyclohexane from the FH of the BR in −O-BR of BOB to produce toluene and CHOA followed by the FH of toluene to get methylcyclohexane and the H + abstraction by CHOA from H···H to obtain CH II . Moreover, NiCs/Al 2 O 3 shows a distinguished recyclability and repeatability.
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高影响因子
FUEL
·
2024
·
IF 6.7
Guang-Hui Liu,Wen-Ao Shi,Jun Li,Han Wang,Ai-Min Wang,Yu-Hong Kang,Yong Gao,Ni Bai,Jie Kang,Chen Shi,Xian-Yong Wei
To produce high-density liquid fuels from lignite, a novel Ni-based bifunctional MCM-41/ β composite zeolite (Ni@ M / β ) is reported for the catalytic hydroconversion (CHC) of lignite-derived aryl ethers to high-yield polycyclic alkanes (PCAs). Ni@ M / β has a three-dimensional channel-type hierarchical porous texture with β as the core and MCM-41 as the shell. Stable Brønsted/Lewis acid sites and abundant internal/inter-zeolite defects also effectively promote the CHC of aryl ethers to PCAs. Under optimal conditions (5 MPa initial H 2 pressure and 160 °C), selectivities of 2-(benzyloxy)naphthalene (BON) and benzyloxybenzene derived PCAs are as high as 76.0 and 90.5 %, respectively, with dimers and trimers dominating. DFT calculation based on electrostatic potential distribution on the van der Waals surface and Mulliken charge distribution of BON and derived oxygenated monomers shows that aromatic intermediates with >C aromatic OH have multiple accessible sites and are easy to bind with cation/radical fragments. Therefore, it is speculated that PCAs are mainly derived from C-C coupling induced by cation/radical fragments after the activation of aromatic α -carbon. In addition, the activation of H 2 to H + , H · , δ+ H ··· H δ- , and H ··· H is mainly attributed to the strong Ni- M / β interaction and abundant defects. The whole CHC process is triggered mainly by the adsorption of H + released by Ni@ M / β at O sites of aryl ethers, and >C aliphatic -O- bridged bond cleavage is dominant. During this period, benzyl cation/radical produced by >C-O- bond cleavage and aromatic α -carbon activation (mainly) is coupled/reformed with adjacent aromatic fragments into corresponding polymers with non-oxygen bridged bonds, which are more easily converted to PCAs. This polycrystalline composite strategy improves the accessibility of large-sized molecules to active centers, and then increases the yields of PCAs, which is attractive for the clean and efficient conversion of lignite-derived oils to high-density liquid fuels.
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高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·Vol. 142
·期 4
·e56399
·
IF 2.7
Wenmin Mu,Chong Tian,Shijie Zhang,Tao Zhuang,Qing Yu,Liang Song,Guiqing Cheng,Zhongwei Wang,Yuxi Han
A fresh phosphorus-containing fireproofing agent (oxybis(4,1-phenylene))bis((2,5-dihydroxyphenyl)(phenyl)phosphine oxide) (ODDPO-HQ) was synthesized by a simple two-step reaction. The effect of ODDPO-HQ on the glass transition temperature ( T g ), crosslinking density, thermal stability, fire resistance, dielectric performances, hydrophobicity, and water absorption of epoxy resin (EP) was studied. EP/ODDPO-HQ containing 1.2 wt% phosphorus not only achieved the vertical burning V-0 grade with a limited oxygen index of 28.9% but also maintained good thermal stability. Compared to unmodified EP, its T g value has only decreased by 7.2°C. Detailed studies revealed that the excellent flame resistance of ODDPO-HQ for epoxies was ascribed to the flame suppression both in the gaseous phase and condensed phase, especially the obvious barrier effect. Although the water uptake of the modified epoxies slightly rose with the content of ODDPO-HQ caused by the reduction of the crosslinking density within the matrix, it did not adversely affect the properties of the polymer. The modified epoxies showed reduced dielectric constant and dielectric loss values, and the contact angle of EP/ODDPO-HQ samples increased as the flame retardant content rose, which might be due to the symmetrical structure of ODDPO-HQ reducing the polarity. Our study presents an easy approach for producing high-performance epoxies.
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高影响因子
FUEL
·
2025
·
IF 7.5
Caitao Chen,Juan Ma,Yakun Tang,Xiaohui Li,Guangbo Liu,Hanyao Song,Yingluo He,Noritatsu Tsubaki,Lang Liu,Ting Liu
Cleaving the aromatic ether C-O bonds of lignite through catalytic hydroconversion (CHC) presents a significant challenge for producing organic chemicals and clean liquid fuels, which are vital for a sustainable future. In this study, we employed a sacrificial template-self-recovery strategy to synthesize highly dispersed and carbon-coated bimetallic catalysts MCo/C (M = Fe, Cu, Ni) for the CHC of Naomaohu coal (NMHC) and lignite-related model compounds (LRMCs). The carbon-coated NiCo bimetallic alloy catalysts, benefiting from the high dispersity of the active components and the synergistic effect between Ni and Co, exhibited excellent hydrogenolysis activity towards diphenyl ether (DPE). DPE conversion reached 100 % over Ni 3 Co 1 /C under optimal conditions (120 °C, 2 MPa H 2 , 2 h). Moreover, Ni 3 Co 1 /C significantly increased the content of arenes and alkanes while reducing the content of oxygen-containing compounds in the NMHC soluble portion (SP), demonstrating its efficient catalytic hydrogenolysis and hydrodeoxygenation capabilities. Density Functional Theory (DFT) calculations revealed that the Ni 3 Co 1 /C catalyst could activate H 2 to generate hydrogen radicals and diatomic active hydrogen, which are the primary hydrogen species involved in the reaction and affect the CHC of DPE. The experimental results can provide a reference for the conversion of lignite into clean liquid fuels.
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高影响因子
BIOMATERIALS
·
2011
·
IF 7.883
Ao Xia,Yuan Gao,Jing Zhou,Chunyan Li,Tianshe Yang,Dongmei Wu,Limin Wu,Fuyou Li
New core–shell structured NaYF 4 :Yb 3+ ,Tm 3+ @Fe x O y nanocrystals , with 20 nm Yb 3+ ,Tm 3+ -co-doped NaYF 4 nanocrystals as a core and 5 nm Fe x O y nanocrystals as a shell, have been synthesized and characterized by TEM and XRD analysis . These core–shell nanocrystals exhibit excellent near-infrared upconversion luminescence (UCL) emission at 800 nm under excitation by a continuous-wave 980 nm laser and superparamagnetic properties with a saturation magnetization (Ms) of ∼12 emu/g. Water-soluble nanocrystals were obtained by surface ligand exchange of oleic acid-coated precursor nanocrystals, and their internalization within living cells has been investigated by laser scanning UCL microscopy. Furthermore, the obtained core–shell nanocrystals have been applied in dual-modality T 2 -enhanced magnetic resonance (MR) and UCL imaging in vivo of the lymphatic system. Moreover, the toxicity of NaYF 4 :Yb 3+ ,Tm 3+ @Fe x O y nanocrystals has also been evaluated by MTT assay, IC50 values, and histological analysis of lymphatic node sections.
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PubMed
高影响因子
Catalysts
·
2024
·Vol. 14
·期 12
·858
·
IF 3.8
Feng Feng,Yajing Liu,Li Yao,Xiuyu Wang
Creatine catalase (CAT), superoxide dismutase (SOD), and NADPH oxidase (NOX) are natural enzyme molecules that play a crucial role in regulating reactive oxygen species (ROS) in biological systems. They maintain life activities and eliminate pathogens by catalyzing various biochemical reactions. However, natural enzymes have some drawbacks in ROS control; they may lose activity under certain environmental conditions, such as high temperatures, extreme pH values, or the presence of organic solvents, which affects their stability and reliability in different applications. The construction of artificial nanozymes is an emerging technology that could probably solve the problems existing in natural enzymes. This study introduces a type of dendritic platinum–iron oxide (DPIO) nanozyme. The unique dendritic structure of this DPIO nanozyme provides a high surface area-to-volume ratio, and the addition of a platinum layer on the surface offers stability, thereby effectively enhancing the catalytic efficiency of producing reactive oxygen species (ROS). The combination of iron-based Fenton reactions and platinum-based Fenton-like reactions in this DPIO nanozyme drastically improves ROS catalytic efficiency. This artificial nanozyme has a high level of biosafety and displays no cytotoxicity. The development of DPIO nanozymes marks a significant advancement in the technology of artificial nanozymes.
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高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-19
·
IF 15.7
Zhang Lei,AL-Ammari Abdulrahman,Zhu Danxuan,Zhang Hongsong,Zhou Peng,Zhi Xu,Ding Weixiao,Li Xinmeng,Yu Qingqing,Gai Yuwen,Ma Xiaoling,Chen Chuntao,Zuo Chao,Zhang Jiaan,Zhu Wanying,Sun Dongping
Vaccines offer prophylactic treatments against atherosclerosis by eliciting effector T cell and antibody responses, which require effective delivery of antigen and adjuvant to activate dendritic cells (DC). Here we show that individual conjugation of antigen p210 and adjuvant CpG oligodeoxynucleotides onto superparamagnetic iron oxide nanoparticles formulates a nanovaccine cocktail that activates DCs for antigen cross-presentation and induction of co-stimulatory signals, cytokines and CD8 + effector/effector memory T cell responses. This nanovaccine modulates the DCs in the draining lymph nodes, activates both CD4 + and CD8 + T cells, elicits memory responses, and induces both anti-p210 IgM and IgG antibodies to suppress atherosclerosis. Lastly, three intradermal vaccinations of this nanovaccine mitigate the atherosclerosis development in the ApoE −/− mice. Our nanovaccine design and preclinical data thus presents a potential candidate for prophylactic treatment for atherosclerosis.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Xue Zhong,Weicheng Jiao,Wenbo Liu,Rongguo Wang,Xiaodong He
Flexible pressure sensors have attracted great interest as they play an important role in various fields such as health monitoring and human–machine interactions. The design of the pressure sensors still faces challenges in achieving a high sensitivity for a wide sensing range, and the interference of water restricts the applications of the sensors. Herein, we developed a graphene–polydimethylsiloxane film combining a hierarchical surface with nanowrinkles on it and a hollow structure. The microstructure design of the composite can be facilely controlled to improve the sensing and hydrophobic performance by tailoring the microsphere building units. Attributed to the irregular surface and hollow structure of the sensing layer, the optimized sensor exhibits a superior sensitivity of 1085 kPa–1 in a 50 kPa linear range. For practical applications, the nanowrinkles on the surface of the microspheres and the polymer coating endow the composite with waterproof properties. Inspired by the dual receptors of the skin, two designed microstructured films can simply integrate into one with double-sided microstructures. The sensing performance and the water-repellence property allow the sensor to detect physiological signals under both ambient and underwater conditions. Furthermore, underwater stimuli detection and communication are demonstrated. This method of fabricating a flexible sensor shows great potential in wearable and robotic fields.
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PubMed
高影响因子
FUEL
·
2024
·
IF 6.7
Yingxiong Zhang,Ting Liu,Yakun Tang,Jingmei Liu,Yue Zhang,Xiaodong Zhou,Xiaohui Li,Lang Liu
The catalytic conversion of oxygen-containing aromatic ring in lignite under mild conditions is crucial to obtain clean liquid fuel. Here, hollow nanosphere Ni 3 P-500–24 catalysts were prepared at a calcination temperature of 500 °C and acid-etching time of 24 h. The porous hollow nanospheres structure could expose more catalytic sites, and the electron-rich nickel exhibited a good catalytic activity. The conversion rate of benzyl phenyl ether (BPE) was 100 % (140 ℃, 1 MPa H 2 , 2 h), and the main products were methylcyclohexane and cyclohexanol, indicating that the catalyst had good catalytic hydrocracking performance. In addition, the catalyst exhibited certain deoxygenation activity and high product selectivity for other oxygen-containing model compounds. For the catalytic hydrogenation of Naomaohu coal (NMHC) soluble portion, the content of alkanes increased from 19 % to 47 %, while the content of oxygen-containing compounds decreased from 56 % to 21 %, which further demonstrate that the catalyst have good catalytic hydrogenation and deoxygenation performance. Density Functional Theory (DFT) calculations showed that the properties of the Ni 3 P-500–24 catalyst was similar to noble metal, which could activate H 2 to produce two kind of active hydrogen: H radical and diatomic hydrogen. The synergistic pathways for the transfer of active hydrogen during the catalytic hydroconversion (CHC) process were analyzed. Above results could provide theoretical guidance for the conversion of lignite into high-quality clean liquid fuels.
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高影响因子
FUEL
·
2024
·
IF 6.7
Fa-Peng Wu,Le-Le Qiu,Yun-Peng Zhao,Zong-Pin Fu,Jing Liang,Jian Xiao,Jian Li,Fang-Jing Liu,Jing-Pei Cao
Hydrogenolysis of β-O-4 linkages in lignin to produce aromatic compounds is attractive but challenging. Currently, external hydrogen source like hydrogen gas or hydrogen-donor solvent is necessary during hydrogenolysis, leading to high cost and low selectivity of products. Herein, a NiCu/Al 2 O 3 catalyst was prepared for self-hydrogen transfer hydrogenolysis (SHTH) of C β -O bond using inherent C α H-OH structure as H-source. A β-O-4 model compound, 2-phenoxy-1-phenethanol, was completely transformed into acetophenone and phenol at 220 ℃ under 1 MPa N 2 for 2h. The SHTH reaction proceeded through a dehydrogenation reaction followed by a hydrogenolysis reaction. Hydrogen radicals released from C α H-OH group generated a “hydrogen pool” on the catalyst surface, which inserted into the formed β-O-4 ketone intermediate to cleave the C β -O bond. The catalyst presented outstanding reusability and universality during the SHTH reaction. Moreover, the methoxy groups at aryl positions impeded the SHTH process, and the steric effect was related to the amount and position of methoxy groups. This study realizes the utilization of structural hydrogen from lignin model compounds for its C β -O bond cleavage , providing an economical and sustainable method toward lignin valorization.
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Ying Wu,Meng Guo,Jie Gao,Jian-Hui Li,Bo-Kun Chen
The active ingredients most commonly employed in sunscreens are compounds containing one or two aromatic rings. Lignin is the most abundant renewable aromatic polymer that has the potential to yield low molecular weight aromatic chemicals when strategically depolymerized. Here, the UV absorbance of a series of monomeric and dimeric lignin model compounds (LMCs) were studied. Specifically, vanillin and ferulic acid demonstrated good absorption in the UVB (280–320 nm) range, while the 5–5 dimer showed efficient absorption in the UVA (320–400 nm) range. Based on this, vanillin, ferulic acid and 5–5 dimer were mixed in pairs and dispersed in the oily isoeugenol to prepare LMC hybrid dispersions. Subsequently, demethylated lignin (DL) was synthesized and used to encapsulate the LMC hybrid dispersions via ultrasonic cavitation to prepare DL-based nano-capsules (DLNCs). The DLNCs were used as the only active ingredient in sunscreens, whose sun protection factor (SPF) value could be up to 55 with a dosage of 10 wt%. Due to anti-photolysis property of DL, the SPF value of DLNCs-based sunscreens increased initially and maintained >8 h under UV irradiation. Additionally, the prepared DLNCs exhibited excellent anti-permeability, antioxidant capacity and biocompatibility, making them a potential substitute for conventional petroleum-based sunscreen agents.
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高影响因子
危险品化学品经营许可证（带存储）