ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 31
·期 24
·2101181
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IF 18.808
Yifei Shen,Xiaohui Shen,Mei Yang,Jiangfeng Qian,Yuliang Cao,Hanxi Yang,Yang Luo,Xinping Ai
Chemical prelithiation is an effective approach to elevate the initial Coulombic efficiency (ICE) and energy utilization of Li-ion battery electrodes. However, this approach fails to operate for the most commonly used graphite (Gr) anode, because all the prelithiation reagents reported so far have a much higher redox potential than Gr (≈0.2 V). Based on ionic solvation and coordination chemistry, for the first time, a new design strategy is proposed for prelithiation solution by selecting a strong electron-donating, sterically hindered, and chemically stable solvent to tune the redox potential of prelithiation reagent and also to prevent the solvent co-intercalation during prelithiation process, thus enabling a successful prelithiation of Gr anodes. By theoretical prediction and experimental evaluation, a chemical prelithiation solution, lithium biphenylide/2-methyl tetrahydrofuran, is successfully developed, which can prelithiate Gr anodes accurately to a desired state in few minutes without destroying the lattice structure of Gr. When the prelithiated Gr anodes (pGr) are paired with the conventional cathodes, the full cells demonstrate significantly improved ICEs and higher energy densities than their counterparts using pristine Gr anodes, showing a great prospect for wide Li-ion battery applications.
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ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Fuyang Jiang,Yi Sun,Kuanxin Zhang,Yongchao Liu,Xuyong Feng,Hongfa Xiang
SiO x is considered to be a promising anode material for lithium-ion batteries (LIBs) due to the high lithium storage capacity. However, the large initial irreversible capacity loss and intensive volume change during cycling hinder its commercial applications. Prelithiation is an effective and convenient strategy to improve the initial Coulombic efficiency (ICE) of SiO x , while incomplete and unstable SEI on the prelithiated anode still results in rapid capacity decay. Herein, through the synergy effect of chemical pre-lithiation process and fluoroethylene carbonate reduction, a compact and stable LiF-rich SEI layer is in-situ formed on the surface of prelithiated SiO x anode. The modified SiO x anode exhibits a high ICE of 90.7% with good cycling performance. When paired with the commercial LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622) cathode, the assemble pre-Li-SiO x /C||NCM622 full cell exhibit a high ICE of 85.7% and stable cycling stability. This work provides a new insight in constructing favorable SEI in pre-lithiation process.
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Journal of Flow Chemistry
·
2021
·Vol. 11
·期 4
·843-853
·
IF 2.786
Jiang Xinxiang,Li Guangxiao,Liu Saier,Song Yang,Su Yuanhai
The process characteristics of two main steps in the preparation of 4-nitrobiphenyl (4-NBP) from 4-nitroaniline (PNA) were clearly revealed by applying two continuous-flow microreactors. The first step was the synthesis of 4-nitrobenzene diazonium tetrafluoroborate (4-NBDT) through the diazotization reaction. The reaction temperature, the residence time, and the molar ratio of different reactants were investigated to achieve optimal reaction conditions with the highest yield of 4-NBDT. Notably, the yield of 4-NBDT reached 97% at 25 °C only in 2.3 s with the optimal molar ratio of HBF 4 , NaNO 2 and PNA (i.e., 2.72:1.05:1). The second step was the Suzuki-Miyaura cross-coupling reaction, in which HNO 3 was used to transform the reaction system into a homogeneous state. The effects of mixing performance, the molar percentage of Pd(OAc) 2 to 4-NBDT, the reaction temperature and the residence time on the Suzuki-Miyaura cross-coupling reaction were investigated systematically. With the molar percentage of Pd(OAc) 2 to 4-NBDT of 1 mol%, the yield of 4-nitrobiphenyl (4-NBP) was optimized to 99% in just 13 min at 25 °C. This study demonstrated the excellent potential of utilizing the continuous-flow microreactor for the diazotization and the following Suzuki-Miyaura cross-coupling reaction.
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BIOCHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 3.978
Tao Xu,Teng Liu,Dawei Jiang,Ziyue Yuan,Xiaoqiang Jia
Persistent organic pollutants (POPs) mainly including polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs), and organochlorine pesticides (OPs), have long-term harmful effects on human health and the environment. In this study, a natural consortium BP-W was attained from oil-contaminated soil using biphenyl as the sole carbon source, which is a relatively simple PAH and can form PCBs under certain catalytic conditions. PCR-DGGE techniques were used to analyze the structure of the consortium BP-W. The results showed that this consortium was composed of Chryseobacterium BP-1, Pseudomonas putida BP-2, Stenotrophomonas BP-3, Achromobacter BP-4, and an uncultured bacterium. The consortium BP-W degraded 99.88 % of 1 g L −1 biphenyl in 72 h. The degradation ratios of 100 mg L −1 naphthalene, phenanthrene, pyrene, and PCB77 in 5 days were 100 %, 97.54 %, 42.26 %, and 26.73 %, respectively. Notably, the consortium BP-W exhibited a high tolerance for these POPs. In the binary-substrate and ternary-substrate systems, the consortium BP-W was still able to rapidly degrade organic substrates. The results of gas chromatography-mass spectrometry showed that biphenyl was completely degraded by BP-W and entered the TCA cycle through the protocatechuic acid pathway, and no other highly toxic metabolites were produced during the degradation process. Thus, this consortium BP-W may have potential utility for the environmental-friendly and cost-effective bioremediation of POPs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Wei Guo,Yao Qin,Cheng Liu,Binbin Guo,Junhua Zou,Zenghong Xie,Ling Wu
This work reports the rapid and effective photocatalytic dechlorination of 3,3′,4,4′-trtrachlorobiphenyl (PCB77) with highly dispersed Pd nanoclusters loaded two-dimensional (2D) TiO 2 (B) nanosheets (Pd/TiO 2 (B)) under visible light irradiation, achieving a dechlorination efficiency of 100 % with H 2 O used as an H-donor source. The ultra-thin TiO 2 (B) nanosheets provide a good platform for studying the dechlorination intermediates/pathways of PCB77 at the molecular level. It is proved that the dechlorination of PCB77 is a stepwise process, in which chlorines at the para positions are much more susceptible than those at the meta positions due to the activation of the C Cl bond in the presence of Pd nanoclusters. Furthermore, in-situ FTIR results of D 2 O absorption suggest that the TiO 2 (B) nanosheets with abundant surface defects greatly promote the activation of water molecules via the formation of surficial complexes by hydrogen bonds. Finally, a synergistic mechanism is proposed for photocatalytic dechlorination of PCB77 over Pd/TiO 2 (B). The study provides an efficient method for complete dechlorination of PCB77 and an in-depth understanding photocatalyzed dechlorination reaction mechanism at the molecular level, which may extend to other photocatalytic dehalogenation reactions of halogenated pollutants.
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 1
·263-275
·
IF 3.186
Wei Jian,Huang He,Luo Qinglong,Liu Na,Wang Xueying,Wang Xuefeng,Zhong Mei,Huang Xueli
Few layer (< 5 layers) MoS 2 mixed with a 1T phase has the characteristics of a large specific surface area and an improved active site distribution. Therefore, it has been increasingly study for the catalytic hydrodesulfurization of polycyclic compounds. In this paper, few-layer MoS 2 with a high proportion of the 1T phase is synthesized by a one-step solvothermal method using a green non-toxic ethanol/water solvent. Results show that few-layer MoS 2 (3–5 layers) with a 1T phase up to 48% can be synthesized in a 50% ethanol solvent. This MoS 2 is used to catalyse the hydrodesulfurization reaction of dibenzothiophene, and the target product conversion rate reaches 84.2%. Among them, biphenyl accounts for 70.2%, phenylcyclohexane accounts for 13.9%, and bicyclohexane accounts for 0.4%. According to the Hansen solubility parameter (HSP) distance Ra, the effects of solvents on the structure and morphology of MoS 2 and the conversion of dibenzothiophene hydrodesulfurization are determined. This work is significant for the synchronous synthetic exfoliation of MoS 2 with a controllable number of layers, a higher ratio of the 1T phase and good catalytic HDS of polycyclic compounds. Graphic Abstract Few layers and high proportion of 1T phase MoS 2 by solvothermal synthesis for catalytic hydrodesulfurization of dibenzothiophene.
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JOURNAL OF CHROMATOGRAPHY A
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2020
·
IF 4.049
Xiaohuan Zang,Yachao Pang,Hongda Li,Qingyun Chang,Shuaihua Zhang,Chun Wang,Zhi Wang
A covalent organic framework modified graphitic carbon nitride (g-C 3 N 4 @TpBD) was synthesized by modifying the graphitic carbon nitride (g-C 3 N 4 ) with a covalent organic framework (COF-TpBD). The synthesis conditions including the mass ratio between g-C 3 N 4 and benzidine (BD), solvent type, reaction temperature and reaction time were optimized. Under the optimal synthetic conditions, a novel spiny dendritic g-C 3 N 4 @TpBD adsorbent was obtained. The g-C 3 N 4 @TpBD was then coated on stainless-steel wire by sol-gel technique and the coated fiber was used for the solid phase microextraction of polycyclic aromatic hydrocarbons prior to gas chromatography-mass spectrometric detection. The established method was successfully applied to determine eight PAHs in six environmental water samples. Under the optimal extraction conditions, a wide linear quantification range for the analytes was obtained from 0.07 to 60.0 ng mL −1 with the coefficients of determination varying from 0.9979 to 0.9998, and the limits of detection (S/N = 3) ranged from 0.02 to 0.05 ng mL −1 . The relative recoveries of the analytes for the six environmental water samples at the spiked concentrations of 0.2, 0.5, 3.0 and 30.0 ng mL −1 were between 83.6% and 118% with the relative standard deviations ranging from 2.4% to 11.3%.
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PubMed
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JOURNAL OF POWER SOURCES
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2021
·
IF 9.127
Xinming Du,Hongyu Zhang,Yongjiang Yuan,Zhe Wang
The ether-bond-free poly(biphenyl piperidine)s are prepared to improve the alkaline stability of the anion exchange membrane (AEMs). At the same time, the construction of micro-phase separation structure is a good way to solve the “trade-off” problem between ionic conductivity and stability of AEMs. In this study, we report a new method for constructing micro-phase separation structures based on “main-chain type” AEMs and a crosslinking strategy that does not sacrifice ion exchange capacity . A series of poly(biphenyl piperidine)s AEMs (PAP–OH–x) are prepared by introducing 2-bromoethanol and 1,6-dibromohexane to form piperidine cationic groups and cross-linked structure. The structure of hydrophilic/hydrophobic phase separation is confirmed by TEM images. The cross-linked membrane of poly(biphenyl piperidine)s (PAP–OH–8%) membrane exhibits high conductivity of 0.081 S/cm with a rational water absorption (55.6%) and low swelling ratio (11.8%) at 80 °C, and also preserves the hydroxide conductivity (89.2% retention) after testing in a 5 M NaOH aqueous solution at 80 °C for 30 days, exhibits high alkaline stability. Furthermore, a single H 2 /O 2 fuel cell with poly(biphenyl piperidine)s (PAP–OH–8%) membrane exhibits the open circuit voltage of 1.02 V and the peak power density of 290 mW/cm 2 at 60 °C.
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Molecular Catalysis
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2020
·
IF 3.687
Lihui Yang,Xiao Zhao,Manjun Lei,Jie Sun,Lei Yang,Yifeng Shen,Qiangqiang Zhao
In this paper, a thermo-responsive Pickering emulsion (PE) is constructed for the esterification reaction in the phase transfer catalysis (PTC) system. Silica nanoparticle modified by alkyl polyoxyethylene ether and tetrabutylammonium bromide (TBAB) is the highly efficient thermo-responsive Pickering emulsifier to stabilize the diisopropyl ketone-in-water emulsion. PEs can keep stable at room temperature for 3 days and demulsify only in the condition of elevated temperature and agitation, which causes the easy product separation and aqueous phase recycling. The adsorption of TBA + and nonionic surfactant via electrostatic interaction and hydrogen bonding, respectively, can increase the hydrophobicity and the emulsifying capacity of silica nanoparticle. The ion-pair of TBA + and reactant anion is generated and can be transferred into the organic phase, initiating the bond-forming reaction. The modifying effect of polyoxyethylene ether is weakened with the increase of temperature due to the loss of the hydrogen bonding interaction, resulting in the demulsification of PEs. Moreover, the cloud point of polyoxyethylene ether is the temperature for the complete separation of two phases. In this PTC system, the conversion rate for the esterification can reach to 92 % and the aqueous phase can be reused at least 5 times without sacrifice of the catalytic activity, demonstrating the potential application in industry.
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JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Xinming Du,Zhe Wang,Hongyu Zhang,Yongjiang Yuan,Hui Wang,Zhenguo Zhang
The diffusion dialysis (DD) process based on AEM is considered for the acid recovery from acid effluents. In this work, the novel self-organized nanostructured cross-linked AEMs based on poly (aryl piperidinium) are synthesized for acid recovery. The cross-linked AEMs are designed by introducing 2-bromoethanol and 1,6-dibromohexane into the hydrophobic poly (biphenyl piperidine)s backbone via Menshutkin reaction, and the self-assembled nanostructure is confirmed by TEM imagines. The acid flux is improved by constructing a micro-phase separation structure and hydrogen bond network. The H-bond networks and cross-linking structure improve the selectivity between the acid and salt system without sacrificing IEC values of AEM. The IEC values of PBP-OH-x AEMs are in the range of 2.18–2.21 mmol/g. The AEMs exhibit high H + dialysis coefficients (U H ), ranging from 0.045 to 0.053 m/h, and have good separation factors (S) in the range of 32–56. The prepared PBP-OH-x AEMs have better DD performance, comparing with the commercial membrane DF-120 (U H = 0.009 m/h, S = 18.5). The novel AEMs based on poly (aryl piperidinium) showed the potential to be used in acid recovery via DD.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Huiyan Li,Gaimei Wang,Kok-Giap Haw,Jialu Li,Huazhen Rong,Hao Ren,Yongyan Deng,Ye Yuan,Guangshan Zhu,Xiaoqin Zou
Xenon is found a wide range of applications in our modern life, and its purification and separation is of paramount importance in industry. For this goal, we have synthesized several porous organic frameworks (POFs) from the perspective of pore chemistry. The prepared materials (CTF-0, PAF-45, PAF-67) show almost identical pore size of ~5.0 Å, appreciable surface areas (528.4–1158.5 m 2 g −1 ), substantial micropore volumes (0.158–0.3 cm 3 g −1 ) and high stabilities (400–600 °C). Adsorption measurements demonstrate that the prepared materials have xenon uptakes in the range of 25.2–62.8 cm 3 g −1 at 1.0 bar and 298 K, and Henry predictions reveal that they are selective for separating xenon from krypton with selectivities of 5.2–8.1. As a representative material, PAF-45 has been tested for xenon separation by the breakthrough experiment, and selectivity of 12.3 for xenon over krypton and xenon capacity of 92.4 mmol kg −1 are obtained.
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APPLIED CATALYSIS A-GENERAL
·
2020
·
IF 5.006
Xiaoting Jing,Zhen Li,Bing Lu,Yuyang Han,Yingnan Chi,Changwen Hu
Compressible monolithic catalysts exhibit remarkable advantages over traditional powder ones, but the fabrication of polyoxometalate (POM)-containing compressible catalyst is rarely explored. Herein, a compressible monolith, PW 12 @GF, has been fabricated by immobilizing H 3 PW 12 O 40 (PW 12 ) catalyst on elastic graphene foam (GF). Moreover, FT-IR and XPS spectra analysis and leaching test reveal that the delocalization of protons on POM occurs during the assembly of PW 12 @GF, and the delocalized protons connect POM and GF into a stable composite. Importantly, biodiesel production is effectively promoted by PW 12 @GF under mild conditions (60 °C) without stirring, and the product can be easily separated from the catalyst by compression. Moreover, its catalytic activity is basically maintained after five cycles. Notably, the catalytic activity of PW 12 @GF (conversion: 97 %) in the heterogeneous system is even comparable to that of homogeneous PW 12 and strong Brønsted acidity and the lipophilic surface of the catalyst account for the excellent performance.
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