Materials Today Energy
·
2021
·
IF 7.311
J. Yang,F. Mo,L. Huang,H. Liang,G. Sun,S. Peng
Black phosphorus/natural graphene (BP/NG) composite electrode material for all-solid-state lithium-ion batteries (ASSLIBs) was fabricated by a facile ball milling method. A C-P bond with characteristics of high ion and electron transfer was constructed, which unlocked the reversible cycling and rate performance of phosphorus. In addition, compounding black phosphorus (BP) with natural graphene (NG) can relieve the large internal stress caused by volume change during cycling and improve the stability of the long cycling and high-rate performance. At current density of 0.5 A g −1 , a high specific capacity of 750 mAh g −1 remained after 100 cycles, whereas at high current density of 1 A g −1 , the BP/NG anode material delivered a reversible capacity of ~300 mAh g −1 . Furthermore, the reaction controlling step of Li x P delithiation was revealed by kinetic measurement. In addition, when coupling BP/NG anode material with TiS 2 to assemble a full solid-state cell, it delivered a high capacity of 400 mAh g −1 after 30 cycles, indicating a potential of further application. This work expanded the candidate of anode materials for ASSLIBs and provided aid for the further application of all-solid-state batteries.
研究领域:
材料科学
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能源存储
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2023
·
IF 20.4
Chengyao Zhao,Yiming Lin,Qiaoyan Lin,Qi Liu,Yujing Liu,Zhongqiu Liu,Anguo Ying
Aqueous zinc-ion hybrid capacitors (ZIHCs) are a promising new type of energy storage device, but there is a plight that the unsatisfactory Zn 2+ storage capability of carbonaceous cathodes limits further application. To address this issue, desolvation strategy is employed to tailor the solvation sheath of Zn 2+ in the ultra-micropores (0.59 nm) nanospheres , where H 3 PO 4 acts as phosphorus source for forming C-P bonds and enhancing C=O bonds to further reduce the desolvation energy barrier. In practical application, a quasi-solid-state flexible ZIHC is constructed, which provides a battery-level energy density (293.4 Wh kg −1 ) at a power density (180 W kg − 1 ) and a remarkable capacity retention of 93.4 % after 10 000 cycles. Electrochemical analyses, DFT calculations and structural characterization reveal that ultra-microporous is proved to be a prerequisite for C-P/C=O that are expected to further deplete solvent molecules within a Zn 2+ solvation sheath. Also, the coupling effect between the strong adsorption of Zn 2+ by C-P/C=O and the hydrophobic effect of C-P play an important role in facilitating desolvation process. This work creates a precedent for the application of ultra-microporous carbon materials in ZHICs and provides a brand-new approach for breaking the bottleneck of the low energy density and poor lifespan of ZHICs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2022
·Vol. 27
·期 22
·7798
·
IF 4.927
Yuelin Xu,Fengxi Li,Jinglin Ma,Jiapeng Li,Hanqing Xie,Chunyu Wang,Peng Chen,Lei Wang
Organophosphorus compounds are the core structure of many active natural products. The synthesis of these compounds is generally achieved by metal catalysis requiring specifically functionalized substrates or harsh conditions. Herein, we disclose the phospha-Michael addition reaction of biphenyphosphine oxide with various substituted β-nitrostyrenes or benzylidene malononitriles. This biocatalytic strategy provides a direct route for the synthesis of C-P bonds with good functional group compatibility and simple and practical operation. Under the optimal conditions (styrene (0.5 mmol), biphenyphosphine oxide (0.5 mmol), Novozym 435 (300 U), and EtOH (1 mL)), lipase leads to the formation of organophosphorus compounds in yields up to 94% at room temperature. Furthermore, we confirm the role of the catalytic triad of lipase in this phospha-Michael addition reaction. This new biocatalytic system will have broad applications in organic synthesis.Keywords:lipase;biocatalysts;promiscuity;C-P bonds;Michael addition reactions
研究领域:
有机化学
·
生物催化
·
酶学
✓ 已验证
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Nuanqin Zhang,Hongwei Sun,Guangming Zhan,Junning Zu,Lizhi Zhang
Glyphosate (PMG) is a globally used broad-spectrum herbicide and receives environmental concerns because of its moderate persistence and potential carcinogenicity. Traditional PMG treatment methods often suffer from the generation of a more toxic and persistent aminomethylphosphonic acid (AMPA) intermediate. Herein, we develop a green method with ferrihydrite (FH) and CaO2 (FH/CaO2) via regulating the coordination of PMG with FH and Ca2+, where the phosphonate group of PMG preferentially binds to FH and its carboxylate side complexes with Ca2+ released by CaO2, forming a FH-PMG-Ca ternary surface complex. This unique ternary complex can redistribute electrons within the PMG molecule for its C–P activation and C–N bond stabilization, favoring the selective C–P bond attack of superoxide radical produced by the Fenton reaction between CaO2-derived H2O2 and FH, thus generating environment-friendly glycine instead of AMPA. The FH/CaO2 process realizes over 99% PMG degradation in industrial wastewater within 1 h, with residual PMG < 0.1 ppm and AMPA < 40 ppb. More importantly, the CaO2 consumption was as low as 3.1 mg of CaO2/mg of PMG, one-fifth those of previously reported CaO2-based counterparts. This study provides an effective and environment-friendly PMG treatment strategy and highlights the importance of surface coordination modes on the degradation pathway of PMG.
研究领域:
环境科学
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污染治理
·
绿色化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jiarun Cheng,Chaojie Lyu,Hangren Li,Jiwen Wu,Yue Hu,Bin Han,Kaili Wu,Mirabbos Hojamberdiev,Dongsheng Geng
An original strategy was reported to manipulate ORR selectivity of N-doped hollow mesoporous carbon spheres (N-HMCS) via heteroatom (P and S) doping. Heteroatom doping can not only modulate electronic structure of N-HMCS and proportion/configuration of doped N, but also regulate ORR pathway. Specifically, rich-graphitic N sites and electron-rich C–P bond domains in N,P-HMCS act as electron donors, making *OOH more unstable and easier to desorb into H 2 O 2 . This severely distorts the sp 2 lattice of graphene, catalyzing a two-electron ORR synergistically. Conversely, a strong interaction between electron-deficient C–S bond domain and *OOH intermediate due to the introduction of highly electronegative S hinders the desorption of *OOH, leading to the breakage of the O–O bond and promoting four-electron ORR along with the rich-pyridinic N receptor site. The reaction activity and kinetics mechanism present a positive correlation with proportion of graphitic N, revealing graphitic N is the primary active site with a much faster electron transfer capacity.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2021
·
IF 4.821
Kunxia Li,Xiujuan Qiao,Haiyan Zhao,Yaping He,Qinglin Sheng,Tianli Yue
In this work, we have synthesized the novel carbon dots-black phosphorus nanohybrid (CDs-BP). And a novel label-free electrochemical aptasensor based on CDs-BP was constructed for ultrasensitive detection of Ochratoxins A (OTA). The morphology and structure of nanocomposite were analyzed by transmission electron microscope, X-ray photoelectron spectroscopy, Zeta potential, et al. The CDs-BP nanohybrid, an excellent carrier for the immobilization of aptamer (Apta), was prepared through C-P bond, resulting in the enhancement of the electrochemical sensing performance for OTA detection. The results showed that the aptasensor had a wide linear range towards OTA (0.1 fg/mL − 10.0 ng/mL) with a low detection limit of 0.03 fg/mL under the optimal conditions. The proposed aptasensor displayed good electrochemical stability and excellent selectivity to OTA detection. Moreover, a satisfactory practical application results were obtained for different actual samples of wheat and grape juice samples. Thus, a new aptasensor was raised based on the CDs-BP nanocompound for the electrochemical detection of contaminants in edible agricultural food.
研究领域:
分析化学
·
纳米技术
·
食品安全
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）