BIORESOURCE TECHNOLOGY
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2021
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IF 9.642
Qiang Chen,Mingzhao Guo,Yuexin Bi,Ge Qu,Zhoutong Sun,Yujun Wang,Guangsheng Luo
This work aims to synthesize S -(4-chlorophenyl)-(pyridin-2-yl) methanol ( S -CPMA) in a green, economic, and efficient way. In the water–cyclohexane liquid–liquid system, recombinant Escherichia coli ( E. coli ) was used as a whole-cell catalyst and retained > 60% of its catalytic activity after five reuse cycles. In situ accumulation of the substrate/product in the organic phase effectively improves substrate tolerance and reduces product inhibition and toxicity. Meanwhile, a microreaction system consisting of membrane dispersion and three-dimensional (3D) bending-microchannel was developed to successfully generate droplet swarms with an average diameter of 30 μm. Large specific surface area provided high mass transfer efficiency between phases. While the analogous reaction in a traditional stirred tank required > 270 min to achieve a yield of > 99%, in this biphasic microreaction system, the yield reached 99.6% with a high enantiomeric excess (ee) of > 99% in only 80 min. Efficient synthesis was achieved by reducing the time by 70%.
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ADVANCED MATERIALS
·
2021
·Vol. 33
·期 16
·2100229
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IF 30.849
Yanxia Wang,Yangyang Lai,Jun Chu,Zichao Yan,Yun-Xiao Wang,Shu-Lei Chou,Hua-Kun Liu,Shi Xue Dou,Xinping Ai,Hanxi Yang,Yuliang Cao
Room-temperature (RT) sodium–sulfur (Na–S) batteries hold great promise for large-scale energy storage due to the advantages of high energy density, low cost, and resource abundance. The research progress on RT Na–S batteries, however, has been greatly hindered by the sluggish kinetics of the sulfur redox reactions. Herein, an elaborate multifunctional architecture, consisting of N-doped carbon skeletons and tunable MoS 2 sulfiphilic sites, is fabricated via a simple one-pot reaction followed by in situ sulfurization. Beyond the physical confinement and chemical binding of polarized N-doped carbonaceous microflowers, the MoS 2 active sites play a key role in catalyzing polysulfide redox reactions, especially the conversion from long-chain Na 2 S n (4 ≤ n ≤ 8) to short-chain Na 2 S 2 and Na 2 S. Significantly, the electrocatalytic activity of MoS 2 can be tunable via adjusting the discharge depth. It is remarkable that the sodiated MoS 2 exhibits much stronger binding energy and electrocatalytic behavior compared to MoS 2 sites, effectively enhancing the formation of the final Na 2 S product. Consequently, the S cathode achieves superior electrochemical performance in RT Na–S batteries, delivering a high capacity of 774.2 mAh g −1 after 800 cycles at 0.2 A g −1 , and an ultrahigh capacity retention with a capacity decay rate of only 0.0055% per cycle over 2800 cycles.
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Materials
·
2021
·Vol. 14
·期 11
·2741
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IF 3.623
Pengcheng Lv,Ruihong Meng,Zhongyang Mao,Min Deng
In this study, the hydrated sodium aluminosilicate material was synthesized by one-step hydrothermal alkaline desilication using fly ash (FA) as raw material. The synthesized materials were characterized by XRD, XRF, FT-IR and SEM. The characterization results showed that the alkali-soluble desilication successfully had synthesized the sodium aluminosilicate crystalline (N-A-S-H) phase of sodalite-type (SOD), and the modified material had good ionic affinity and adsorption capacity. In order to figure out the suitability of SOD as an adsorbent for the removal of ammonium and phosphorus from wastewater, the effects of material dosing, contact time, ambient pH and initial solute concentration on the simultaneous removal of ammonium and phosphorus are investigated by intermittent adsorption tests. Under the optimal adsorption conditions, the removal rate of ammonium was 73.3%, the removal rate of phosphate was 85.8% and the unit adsorption capacity reached 9.15 mg/L and 2.14 mg/L, respectively. Adsorption kinetic studies showed that the adsorption of ammonium and phosphorus by SOD was consistent with a quasi-secondary kinetic model. The adsorption isotherm analysis showed that the equilibrium data were in good agreement with the Langmuir and Freundlich model. According to thermodynamic calculations, the adsorption of ammonium and phosphorus was found to be a heat-absorbing and spontaneous process. Therefore, the preparation of SOD by modified FA has good adsorption properties as adsorbent and has excellent potential for application in the removal of contaminants from wastewater.Keywords:N-A-S-H;sodalite;simultaneous removal;ammonium;phosphorus
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Polymers
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2020
·Vol. 12
·期 11
·2640
·
IF 3.426
Peng Dong,Jing Feng,Sujuan Li,Tingli Sun,Qingshan Shi,Xiaobao Xie
Starting from primary amine bearing cyclic carbonatetert-butyl-(2-oxo-1,3-dioxan-5-yl) carbamate (TBODC) and caprolactone (CL), amphiphilic poly(caprolactone-ran-amino trimethyl carbonate)s (P(CL-ran-ATC)s) random copolymers with controlled molecular weight and composition were synthesized via ring opening polymerization (ROP) and deprotection, using stannous octoate (Sn(Oct)2) as catalyst and benzyl alcohol (BnOH) as initiator. Therefore, hydrophilic/lipophilic ratio (HLR) of the P(CL-ran-ATC)s copolymers can be finely adjusted by the feed ratio of TBODC and CL. The antimicrobial activity againstStaphylococcus aureus(S. aureus) andEscherichia coli(E. coli) of P(CL-ran-ATC)s were proportional to HLR, and P(CL-ran-ATC)s presented more vigorous bactericidal activity towardsS. aureus. The minimum inhibitory concentration (MIC) values of P(CL-ran-ATC 50.9%) are 2000 μg mL−1and 3000 μg mL−1forS. aureusandE. coli. While P(CL-ran-ATC 50.9%) exhibited deficient hemolytic activity as 1.41%. In addition, the P(CL-ran-ATC)s showed extremely low cytotoxicity towards fibroblast L929 cells.Keywords:cyclic carbonate;primary amine;poly(ester-carbonate)s;antimicrobial activity;low hemolysis and cytotoxicity
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OPTICAL MATERIALS
·
2020
·
IF 2.779
Xiaoshuo Zhang,Chunhua Li,Sheliang Zhao,Huiyun Pang,Yong Han,Xueli Luo,Wenzhi Tang,Zhonghong Li
Novel S-doped silicon quantum dots (S-SiQDs) were prepared by l -cysteine doped silicon quantum dots (SiQDs) for fluorescent detecting Fe 3+ in water. The as-prepared S-SiQDs sensor with an average diameter of 4.77 nm possessed richness of –NH 2 , endowing good water solubility and strong blue fluorescence. The quantum yield (QY) of ~66% was abtained when S-SiQDs exited at 345 nm. The synergistic effect of electron transfer that the electron of –NH 2 on S-SiQDs surface transfer to 3d unoccupied obrials of Fe 3+ , inner filter effectaccounted for fluorescence quenching. The probe possessed a relative wide liner range from 1 μmol/L to 20 μmol/L with the limit of detection (LOD) of 0.21 μmol/L to detecte Fe 3+ . The as-prepared S-SiQDs sensor could sensitively and selectively detect Fe 3+ in real water samples with satisfied recoveries of 90%–106%, which presented its potential applicability in the environmental fields.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Baofang Zhang,Renlian Chen,Zefan Yang,Yingxin Chen,Lihua Zhou,Yong Yuan
The heteroatom-doped porous carbon material as an alternative to commercial Pt/C catalysts in oxygen reduction reaction has attracted extensive attention. In this study, the rapeseed meal-based material (ARM-900) prepared by carbonization with high temperature and activation with ZnCl 2 had a porous structure and was doped with N and S heteroatoms. Compared to commercial Pt/C catalysts (onset potential of 0.95 V vs. RHE and limiting diffusion current of −5.7 mA cm −2 ), ARM-900 demonstrated excellent electrocatalytic performance with an onset potential of 0.98 V vs. RHE and limiting diffusion current of −8.1 mA cm −2 in O 2 saturated 0.1 M KOH solution. Meanwhile, ARM-900 had higher durability and more superior methanol tolerance than Pt/C catalyst. The excellent ORR performance of ARM-900 was derived from the formation of abundant pore structure and the doping of the autochthonous N and S heteroatoms. MFCs with ARM-900 as the cathode had the maximum power density of 808 mW/m 2 , which was obviously better than Pt/C (709 mW/m 2 ). This study provided an environment-friendly and effective strategy for the reuse of rapeseed meal and the preparation of N and S-doped non-metallic ORR catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Yutong Luo,Jiaheng Qin,Guangxue Yang,Sha Luo,Ziming Zhao,Ming Chen,Jiantai Ma
The rational design and fabrication of distinctive coordination sites is an attractive and challenging approach to develop electrocatalysts with superior activity toward oxygen evolution reaction (OER). Constructing N-doped carbon shells coordinated with transitional metal composites can greatly enhance the OER activity of electrocatalysts. Herein, a facile electrochemical-pyrolysis strategy is applied to synthesize NiS/C 3 N 4 composite with N-Ni-S coordination sites by in-situ crystallization on copper foam (CF). A detailed characterization, especially synchrotron-based X-ray absorption fine structure (XAFS) clearly unravels the N-Ni-S coordination mode is successfully formed. As a result, NiS/C 3 N 4 presents excellent OER performance with a low overpotential of 334 mV at a current density of 10 mA cm −2 , a Tafel slope of 45 mV dec −1 , and robust electrochemical stability for 50 h in basic media, outperforming some recently reported conventional transitional metal electrocatalysts. The outstanding electrocatalytic performance of NiS/C 3 N 4 mainly originates from the N-Ni-S coordination sites, which can provide abundant catalytic active sites, facilitate charge transfer, and enhance electronic conductivity. Furthermore, by tuning the two important experimental parameters of electrodeposition potential and electropolymerization time, the relationship between morphology and electrocatalytic performance of catalysts is deeply explored. This work demonstrates the validity of improving electrocatalytic performance by elaborately tailoring the coordination sites, thereby opening up an applicable and inspiring avenue forward in the design of advanced electrocatalysts for water splitting.
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JOURNAL OF MEMBRANE SCIENCE
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2020
·
IF 7.183
Diao Yuan,Yajun Qin,Songsong Li,Shenghua Du,Yaoyao Xu,Qiang Weng,Pei Chen,Xinbing Chen,Zhongwei An
A novel difluoro aromatic monomer DFTMTE is prepared, which contains five pendant ionizable methoxy and crosslinkable ethanedione groups. Block copolymers are developed via block copolycondensation of the monomers DFTMTE, 4,4′-difluorodiphenyl sulfone and 4,4′-diphenol. Sulfonated block ionomers are obtained via the following demethylation and nucleophilic substitution of the copolymers . The ionomer membranes with ion exchange capacity (IEC) of 1.80–2.16 mequiv. g −1 display high conductivity of 234–319 mS cm −1 at 80 °C and large maximum power density of 1730–2140 mW cm −2 , which is obviously larger than Nafion 212 (117 mS cm −1 and 1350 mW cm −2 ) in the same condition. Their enhanced performances are attributed to excellent microphase separations caused by block copolymer structures and multiple sulfonated side-chains integrating both rigid aromatic and flexible aliphatic units. Meanwhile, crosslinking further improves the balance among the properties of the membranes. For example, CB1SP having IEC of 1.80 mequiv. g −1 displays high comprehensive performance because of DFTMTE units and crosslinking structures, wherein low membrane swelling below 15% at 80 °C, large conductivity of 234 mS cm −1 , high maximum power density of 1730 mW cm −2 and good stability of the membrane electrolyte assembly indicate a high potential in the application of fuel cell.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2020
·
IF 3.807
Yingjie Chen,Zhihao Shi,Shanshan Li,Jianguang Feng,Beili Pang,Liyan Yu,Wenwu Zhang,Lifeng Dong
Heterogeneous nanoparticles with synergistic effects between different composites are potential catalysts with bifunctional catalytic activity for oxygen reduction (ORR) and oxygen evolution reaction (OER). Herein, heteroatoms such as N and S are doped into graphene substrates to improve catalytic activity and structural stability of Ag-MnFe 2 O 4 nanoparticles. Interestingly, these particles keep a primarily heterogeneous structure for their assembly on N, S-codoped graphene (NSG), while Ag domains shrink on S-doped graphene (SG) or N-doped graphene (NG). Subsequently, Ag-MnFe 2 O 4 /NSG shows the best bifunctional catalytic activity due to the improved stability of Ag-MnFe 2 O 4 NPs on NSG and enhanced bonding energy between supports and particles. The Koutecky-Levich plots confirm a major four-electron reaction pathway for the ORRs on Ag-MnFe 2 O 4 /NSG. Meanwhile, Ag-MnFe 2 O 4 /NSG exhibits higher stability and better methanol tolerance than commercial Pt/C. Therefore, Ag-MnFe 2 O 4 /NSG with bi-functional catalytic activity for ORR and OER is a promising non-Pt catalyst candidate.
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CARBOHYDRATE POLYMERS
·
2020
·
IF 7.182
Shixin Liu,Xiang Cai,Wei Xue,Dong Ma,Wu Zhang
We developed a co-delivery system of nitric oxide (NO) and antibiotic for the antibiotic-resistant bacterial infection therapy. The NO could disperse the bacterial biofilms and convert the bacteria into an antibiotic-susceptible planktonic form. Using the chitosan-graft-poly(amidoamine) dendrimer (CS-PAMAM) as the co-delivery system, methicillin (MET) and NO were conjugated successively to form CS-PAMAM-MET/NONOate. The positive CS-PAMAM could efficiently capture the negatively charged bacteria and PAMAM provide abundant reaction points for high payloads of NO and MET. The CS-PAMAM-MET/NONOate displayed effective and combined antibacterial activity to the E. coli and S. aureus . Particularly, for the MET-resistant S. aureus (MRSA), the CS-PAMAM-MET/NONOate displayed the synergistic antibacterial activity. In vivo wound healing assays also confirmed that CS-PAMAM-MET/NONOate could heal the infection formed by MRSA and then accelerate the wound healing effectively. Moreover, CS-PAMAM-MET/NONOate showed no toxicity towards 3T3 cells in vitro and rats in vivo , providing a readily but high-efficient strategy to drug-resistant bacterial infection therapy.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Hairus Abdullah,Noto Susanto Gultom,Hardy Shuwanto,Worku Lakew Kebede,Dong-Hau Kuo
Zn(O,S) has been successfully doped with different amounts of Ho and characterized with X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), diffuse reflectance spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), electrochemical impedance spectroscopy (EIS), and transient photocurrent (TPC). The as-prepared Ho-doped Zn(O,S) catalysts with different Ho amounts are evaluated for hydrogen evolution reaction. The catalyst with the best performance in evolving hydrogen is further utilized to hydrogenate 4-nitrophenol (4-NP) to 4-aminophenol (4-AP). It is found that doping with Ho obviously enhanced charge transfer and photoresponse properties of the catalyst. Therefore, the modified Zn(O,S) can optimally evolve hydrogen by 18 624 μmol/g, which is 20% higher than that of pristine Zn(O,S). Subsequently, the in situ generated hydrogen ions on catalyst surfaces also play an important role as a hydrogen source to hydrogenate 4-NP to 4-AP without any reducing agents such as NaBH4, which is commonly used as a hydrogen source. As Ho is doped in the lattices of Zn(O,S), it acts not only to separate photocarriers and to enhance the charge transfer but also to shorten the diffusion time of nitrophenolate ions to catalyst surfaces for further photocatalytic hydrogenation reaction (PHR) process. A plausible PHR mechanism has been provided to elucidate the great performance of Ho-modified Zn(O,S) for photocatalytic hydrogenation.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Jingyu Lei,Jiahang Chen,Huiming Zhang,Ahmad Naveed,Jun Yang,Yanna Nuli,Jiulin Wang
Sulfurized pyrolyzed poly(acrylonitrile) (S@pPAN) demonstrates high sulfur utilization, no polysulfide dissolution, no self-discharge, and extremely stable cycling. Its precursor, PAN, directly determines the performances of cathode materials, including the sulfur content and its utilization for S@pPAN composite materials. Adopting PAN with the molecular weight approaching 550,000 as the precursor, the sulfur content in S@pPAN approaches 55 wt %, and its reversible specific capacity was 901 mAh g–1(composite) at 50 °C with sulfur utilization over 98%. Moreover, it enabled stable cycling and excellent high rate capability with a specific capacity of 645 mAh g–1 at 5 C. These significantly enhanced electrochemical properties are mainly due to the high molecular weight of the PAN precursor, which provides more space to accommodate amorphous sulfur, along with improved interfacial resistance of S@pPAN.
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