FUEL
·
2021
·
IF 6.609
Mingxing Zhao,Jun Hu,Shiliang Wu,Liu Yang,Xue An,Peng Yuan,Ping Lu
Cyclohexanols, promising oxygenated fuel additives and value-added chemicals, can be obtained by hydrodeoxygenation (HDO) of lignin-derived phenolics. Here, an N-doped bimetallic RuCoN x /NC catalyst was facilely prepared for HDO by direct pyrolysis of chitin impregnated with precursors of Ru and Co. Characterization of RuCoN x /NC with N 2 sorption, scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and NH 3 temperature-programmed desorption (NH 3 -TPD) reveal that the metallic particles of electron-deficient Ru species and electron-enriched Co species were uniformly anchored on the micro-mesoporous N-doped carbon matrix with high dispersion and nano-scale size. The abundant accessible active sites and continuous spillover of H from Ru to Co make RuCoN x /NC an excellent HDO catalyst. 4-Propylguaiacol, a typical phenolic compound from lignin degradation, was hydrodeoxygenated into 92% 4-propylcyclohexanol over RuCoN x /NC at 210 ℃. With temperature increasing, propylcyclohexane became the major product, possessing 95% selectivity at 280 °C after 6 h. Reusability tests show that RuCoN x /NC can be recycled four times without the loss of conversion and initial selectivity. HDO of other phenolic compounds confirms the general applicability of RuCoN x /NC.
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高影响因子
Molecular Catalysis
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2021
·
IF 5.062
Junyi Liu,Xianxiang Liu,Qiong Xu,Dulin Yin
A series of highly active and ortho -position selective catalysts based on (α-Fe 2 O 3 ) 1- x (V 2 O 5 ) x catalysts were proposed for the C -methylation of phenol with methanol. The (α-Fe 2 O 3 ) 1- x (V 2 O 5 ) x catalysts were synthesized by coprecipitation method of Fe and V elements and microwave drying. The chemical composition, material structure, acid-base properties, and structure-activity relationship of (α-Fe 2 O 3 ) 1- x (V 2 O 5 ) x catalysts were systematically analyzed by the techniques of XRD, XPS, TEM, N 2 adsorption-desorption, Raman, UV-Vis, ESR, NH 3 /CO 2 -TPD and Pyridine-IR. The (α-Fe 2 O 3 ) 1- x (V 2 O 5 ) x catalysts have the double advantages of high activity and high stability for the methylation of phenol due to the high BET surface area, large total pore volume, dispersive active sites and enhanced acid-base property. o -cresol and 2,6-xylenol were the main products, and nearly 100% selectivity to the ortho -position of phenol and 90% selectivity to o -cresol were obtained. Furthermore, the (α-Fe 2 O 3 ) 1- x (V 2 O 5 ) x catalysts possess long lifetime over 2500 h and high activity at a weight hourly space velocity of 1.6 h −1 compared with the microwave-dried α-Fe 2 O 3 catalyst. The doping of vanadium improves the activity and stability of α-Fe 2 O 3 catalyst, which attributes to the modification of catalyst structure, especially the improvement of acid-base centers and oxygen vacancy. Recently the (α-Fe 2 O 3 ) 1- x (V 2 O 5 ) x catalysts have been stably and efficiently applied in industry for the methylation of phenol.
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高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Xinyao Zou,Chao Ma,Ang Li,Zhan Gao,Zulipiya Shadike,Kun Jiang,Junliang Zhang,Zhen Huang,Lei Zhu
Electrochemical conversion of CO2 to the syngas hybrid with the Fischer–Tropsch (FT) process is a promising way to produce synthetic fuels from renewable energy sources. The product distribution in liquid hydrocarbons produced by FT synthesis has strong dependence on the CO/H2 ratio of the syngas feedstock. Herein, we demonstrated the feasibility of tuning the CO/H2 ratio at a wide range by developing nanoparticle-assisted Ni–Co binary single-atom catalysts for electrocatalytic production of syngas. By controlling the elemental proportion of Ni–Co in the composite catalysts, electrochemical reduction of CO2 to syngas with a tunable CO/H2 ratio from 0.3 to 27.6 was achieved. For the binary catalysts with a Ni–Co ratio of 1:1, the CO/H2 ratio maintains at 1.3–1.5 in a broad potential range from −0.59 to −0.83 V versus reversible hydrogen electrode (RHE) and the total current density reaches ∼32.2 mA/cm2 at −1.0 V versus RHE. The promotion effect of nanoparticles on Ni–Co single-atom catalysts was validated by partial removal of nanoparticles and further density functional theory (DFT) calculations. As revealed by DFT calculations, nanoparticles incorporated in single-atom sites take essential roles in facilitating the adsorption of CO2 and the formation of *COOH. The origin of CO2RR and hydrogen evolution reaction reactivities can be identified as Ni–N4 and Co–N4 single-atom sites, respectively. The dual active sites allow the facile control of the CO/H2 ratio of electrochemical converted syngas, and it will be beneficial to downstream production of diverse chemicals.
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高影响因子
Polymer-Plastics Technology and Materials
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2021
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IF 2.371
Dina F. Katowah,Gharam I. Mohammed,Waheed A. Adeosun,Abullah M. Asiri,Mahmoud A. Hussein
This paper reports an electrochemical sensor developed based on cross-linked polyaniline/(chitosan-oxidized single-walled carbon nanotube-graphene oxide/copper oxide) nanocomposite (C-PANI/(OXSWCNTs-GO-CS)/CuO NCs) for detection of a 4-chlorophenol (4-CP). The NCs synthesized by an in-situ chemical polymerization method and characterized by various techniques include XRD, FTIR, SEM-EDX, HR-TEM, TGA-DTG, DTA and cyclic voltammetry. A 4-CP selective electrochemical sensor was fabricated by coating a glassy carbon electrode (GCE) with synthesized NCs. The experimental results reported here displayed the good electrochemical property toward 4-CP oxidation with a detection limit of 0.13 µM (S/N = 3) and good current stability. It also had an impressive percent recovery of the spiked 4-CP in real environmental samples. The improved sensing performances were attributed to the formation of the network structure of C-PANI/(OXSWCNTs-GO-CS)/CuO NCs. Therefore, this study presents a sensitive and promising 4-CP electrochemical sensor for water quality management and human health protection.
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高影响因子
Journal of Water Process Engineering
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2021
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IF 5.485
Wen Huang,Yaxin Tang,Xueping Zhang,Ze Luo,Jianqiang Zhang
The pollution problem of livestock manure generated by the rapid development of farming industry is becoming more and more serious, and its conversion into functional materials through a new way is of great practical significance for its resource utilization. For the first time, nano zero-valent iron (nZVI)/biochar composites (Fe-RMC-850) were prepared by carbonizing Fe 3 O 4 -rabbit dung and used to activate PMS for degradation of sulfamethoxazole (SMX). The results showed that Fe-RMC-850 had high catalytic activity due to its rich pore, high graphitization and defective structure. When the dosage of Fe-RMC-850 and PMS were 0.3 g/L and 0.25 g/L respectively, the degradation rate of SMX could reach 100% within 20 min, and it still showed good catalytic stability after 5 cycles of experiments. The radical quenching, EPR and XPS results showed that radical and nonradical pathways acted synergistically in the degradation of SMX, in which nZVI, Fe 2+ -biochar and pyridinic N were used as the main active sites of the radical pathway. The nonradical pathway was attributed to the generation of C-O and COO by the oxygen-containing functional groups on the biochar surface. Moreover, the inherent P atoms formed P C and CPO 3 /C 2 PO 2 , thereby producing defective structures, while the graphitic carbon layer provided good electron transfer sites. Consequently, this study provides a nZVI-rabbit manure biochar composite PMS catalytic material with high organic pollutant degradation efficiency and offers a new option for the resource utilization of manure sources.
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高影响因子
ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Jilin Yuan,Ming Chen,Wenhao Xiang,Chuanbao Xiao,Nianbing Zhong,Qiang Liao
Rapid and continuous degradation of toxic organic pollutants and conversion to microalgae biomass are attracting enormous interest for resource recovery and wastewater treatment. Aiming toward this goal, we develop and demonstrate a novel photocatalytic-biological system in which photocatalytic optical hollow fibers coated with the N-doped TiO2 photocatalyst and a Scenedesmus obliquus biofilm cooperatively convert phenol to microalgae biomass. The photocatalytic optical hollow fibers exhibit high UV–visible photocatalytic activity to rapidly degrade phenol and emit visible light for biofilm growth, lipid synthesis, and O2 production. O2 produced as an electron acceptor is transferred to the surface of the photocatalytic optical hollow fibers, limiting electron–hole recombination and generating reactive oxygen species such as •OH and •O2–. Upregulation of nicotinamide adenine dinucleotide + hydrogen and adenosine triphosphate and enrichment of Rhodococcus and Pseudomonas in the biofilm enhance the resistance to phenol toxicity, maintain rapid and stable biofilm growth, and increase lipid content. This photocatalytic-biological system rapidly and sustainably converts phenol to microalgae biomass.
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高影响因子
CHINESE JOURNAL OF POLYMER SCIENCE
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2021
·Vol. 40
·期 1
·56-66
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IF 3.603
Sun Ya-Jing,Cheng Xiao-Xiao,Miao Teng-Fei,Ma Hao-Tian,Zhang Wei,Zhu Xiu-Lin
Polymerization-induced chiral self-assembly (PICSA) is an efficient strategy that not only allows the construction of the supramolecular chiral assemblies in a controlled manner but also can regulate the morphology in situ. Herein, a series of azobenzene-containing block copolymer (Azo-BCP) assemblies with tunable morphologies and supramolecular chirality were obtained through the PICSA strategy. The supramolecular chirality of Azo-BCP assemblies could be regulated by carbon dioxide (CO 2 ) stimulus, and completely recovered by bubbling with Ar. A reversible morphology transformation and chiroptical switching process could also be achieved by the alternative 365 nm UV light irradiation and heating-cooling treatment. Moreover, the supramolecular chirality is thermo-responsive and a reversible chiral-achiral switching was successfully realized, which can be reversibly repeated for at least five times. This work provides a feasible strategy for constructing triple stimuli-responsive supramolecular chiral nano-objects in situ .
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高影响因子
Polymer Chemistry
·
2021
·Vol. 13
·期 1
·80-84
·
IF 5.582
Wei Chen,Peng Liu
The ultrasound-mediated approach has attracted attention for enhanced localized drug delivery in tumor chemotherapy. Here, well-defined PEGylated dendritic polyurethane (Ph-DPU-PEG) was synthesized as unimolecular micelles with a hydrophobic core via a facile one-pot method for ultrasound-triggered localized drug delivery. The chemotherapeutic drug could be encapsulated in the hydrophobic cores, and the drug-loaded micelles (DOX@Ph-DPU-PEG) were obtained as nanomedicine, which would hardly release the drug without ultrasound, regardless of the acidity of the releasing media. However, they showed an excellent ultrasound-triggered intracellular drug release performance, with a cumulative drug release of 81.6% in the simulated tumor intracellular microenvironment within 12 h. Furthermore, the ultrasound-triggered intracellular drug release was revealed with the CLSM technique and an enhanced tumor growth inhibition was achieved on the HepG2 cells compared to free DOX.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Wenyang Fu,Zhongzheng Hu,Yang Zheng,Pei Su,Qizhan Zhang,Yongli Jiao,Minghua Zhou
Compared to traditional haber–bosch process for synthetic ammonia, electrochemical reduction of nitrate to ammonia (ERNA) offers a promising and sustainable technology to generate ammonia at ambient temperature. However, the performance of ERNA is impeded by lacking of sound strategy for designing high-performance electrocatalyst. Here, a Cu based electrode with Cu 2 O/Cu interface was prepared by pulse electrodeposition and electroreduction, achieving the fast rate constant of 0.14 min −1 for reducing nitrate with a high ammonia yield rate of 2.17 mg cm -2 h −1 (faradaic efficiency: 84.36%) and ammonia selectivity of 94.4% at −0.25 V vs. RHE. Particularly, density functional theory (DFT) calculations for the adsorption energy indicated that Cu 2 O/Cu interface alleviated adsorption energy of NO 2 - from −2.02 eV (pure Cu) to −1.59 eV, improving surface diffusion of adsorbed NO 2 - . And DFT calculations for electronic structure implied that Cu 2 O/Cu interface upshifted the d band center of Cu (-2.25 eV vs. −2.48 eV of pure Cu), boosting electron transfer to NO 3 - . Additionally, in-situ infrared spectroscopic analysis confirmed vital intermediates of NO 2 - and NH 2 OH on Cu 2 O/Cu to identify reaction pathway and Gibbs free energy diagram clarified this interface decreased reaction barrier of crucial step (reducing *NO 2 to *NO) from 0.31 eV (pure Cu) to −0.77 eV for the enhancement of ERNA. Thereby, these findings demonstrated that Cu 2 O/Cu interface tunes mobility of NO 2 - and electron transfer to NO 3 - on Cu based electrocatalyst is an efficient method to promote performance of ERNA with high efficiency and rate.
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Liying Wu,Zhiqiang Sun,Yufei Zhen,Shishu Zhu,Chen Yang,Jing Lu,Yu Tian,Dan Zhong,Jun Ma
Ubiquitous oxygen vacancies (Vo) existing in metallic compounds can activate peroxymonosulfate (PMS) for water treatment. However, under environmental conditions, especially oxygenated surroundings, the interactions between Vo and PMS as well as the organics degradation mechanism are still ambiguous. In this study, we provide a novel insight into the PMS activation mechanism over Vo-containing Fe–Co layered double hydroxide (LDH). Experimental results show that Vo/PMS is capable of selective degradation of organics via a single-electron-transfer nonradical pathway. Moreover, O2 is firstly demonstrated as the most critical trigger in this system. Mechanistic studies reveal that, with abundant electrons confined in the vacant electron orbitals of Vo, O2 is thermodynamically enabled to capture electrons from Vo to form O2•– under the imprinting effect and start the activation process. Simultaneously, Vo becomes electron-deficient and withdraws the electrons from organics to sustain the electrostatic balance and achieve organics degradation (32% for Bisphenol A without PMS). Different from conventional PMS activation, under the collaboration of kinetics and thermodynamics, PMS is endowed with the ability to donate electrons to Vo as a reductant other than an oxidant to form 1O2. In this case, 1O2 and O2•– act as the indispensable intermediate species to accelerate the circulation of O2 (as high as 14.3 mg/L) in the micro area around Vo, and promote this nano-confinement electron-recycling process with 67% improvement of Bisphenol A degradation. This study provides a brand-new perspective for the nonradical mechanism of PMS activation over Vo-containing metallic compounds in natural environments.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Lingjue Sun,Dongsheng Xu,Yuan Shen,Jacques Crommen,Qiqin Wang,Zhengjin Jiang
Zwitterionic super-hydrophilic polymeric monoliths showed fascinating attributes because of their excellent biocompatibility, hydrophilicity, and antifouling properties. However, their commercial developments are limited by their tedious preparation process and unsatisfactory performance. 1-Carboxy- N -methyl- N -di(2-methacryloyloxyethyl)methanaminium inner salt (CBMAX), an important zwitterionic functional monomer , which exhibits excellent hydrophilicity and extremely low protein adsorption from undiluted serum. However, no carboxybetaine based monolith has been reported to date. In this study, a rapid photo-assisted generation strategy based on a sole-monomer system (CBMAX being simultaneously used as monomer and crosslinker) was proposed for preparing versatile hyper-crosslinked zwitterionic carboxybetaine polymers in capillaries within only 5 min. It is significantly faster than the conventional sole-monomer (1 h) and multi-monomer system (over 12 h) via thermally-initiated polymerization approach. Moreover, a high column efficiency of 82,000 plates/m, abundant electrostatic and hydrophilic interactions were achieved on the novel monolith due to the unique advantages of carboxybetaine. These excellent features were beneficial for the high-performance separation of various bioactive compounds (including nucleotide bases, phenols, benzoic acid and its derivatives, urea and allantoin) on this monolith. It is worth noting that this zwitterionic monolith exhibited good anti-protein adsorption ability as well as excellent enrichment capacity for N -glycopeptides from hIgG tryptic digest. In summary, the proposed photo-assisted generation strategy based on sole-monomer CBMAX is very successful and opens up a promising solution for the commercial development of zwitterionic super-hydrophilic polymeric monoliths.
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高影响因子
ACS ES&T Water
·
2021
·
IF 0
Yangyi Xiao,Chenxing Li,Xiaojiao Zhou,Ningyao Tao,Miaomiao Ye
Recently, seawater desalination based on interfacial solar heating has attracted attention because of its environmental protection and high photothermal conversion efficiency. However, the high air–water interface temperature may cause freshwater quality safety risks because the volatile organic compounds (VOCs) in seawater are more likely to evaporate and condense into freshwater. In this work, typical VOCs (phenol) were prevented from entering into the condensed freshwater by using activated persulfate to take full advantage of interfacial solar distillation. The results showed that the addition of both peroxodisulfate (PDS) and peroxymonosulfate (PMS) could effectively reduce the concentration of phenol in condensed freshwater. The phenol’s distillation concentration rate (RD) was reduced from 74.4% to 14.3% with PMS and 20.5% with PDS. The Cl– was the main factor for activation of PMS, while carbon black, light, and heat were the main factors for activation of PDS. Meanwhile, PMS is better suited for removing VOCs due to its lower oxidant dosage and chlorinated disinfection byproducts compared with PDS. Finally, when real seawater samples were used as the source water for solar distillation, the water quality of typical indicators was lower than the limits set by Drinking Water Quality in China, US EPA, and WHO.
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危险品化学品经营许可证（带存储）