Nano Research
·
2023
·Vol. 16
·期 11
·12697-12705
·
IF 9.9
Gao Xinshuang,Zheng Jia-jia,Li Hanbo,Cai Rui,Gao Xingfa,Wu Xiaochun
Nanozymes, as a novel form of enzyme mimics, have garnered considerable interest. Despite overcoming the main disadvantages of their natural analogs, they still face challenges such as restricted mimic types and low substrate specificity. Herein, we introduce a reactive ligand modification strategy to diversify enzyme mimic types. Specifically, we have utilized helical plasmonic nanorods (HPNRs) modified with para -nitrothiophenol (4-NTP) to create an oxygen-sensitive nitroreductase (NTR) with light-controllability. HPNRs act as a light-adjustable source of nicotinamide adenine dinucleotide/nicotinamide adenine dinucleotide phosphate (NAD(P)H), providing photon-generated energetic electrons to adsorbed 4-NTP molecules. In the presence of O 2 , the activated 4-NTP transfers the captured electron to the adsorbed O 2 , mimicking the electron transfer process in its natural counterpart. This enhanced O 2 activation notably boosts the oxidative coupling of para -aminothiophenol (4-ATP). Density functional theory (DFT) calculations reveal that hot electrons injected into the lowest unoccupied molecular orbital (LUMO) energy level of 4-NTP can be transferred to that of molecular oxygen. In conclusion, our findings underline the potential of the reactive ligand modification strategy in developing new types of enzyme reactions, which opens up promising avenues for the enhancement and diversification of nanozyme functionalities.
研究领域:
生物化学
·
纳米生物学
·
催化科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Qi Chen,Cheng Liu,Rui Liu,Yidong Hou,Jinhong Bi,Jimmy C. Yu,Ling Wu
A series of 2D/2D MoS 2 /Bi 2 WO 6 S-scheme heterojunctions consisting of ultrathin MoS 2 nanosheets (MS, 1.6 nm) and ultrathin Bi 2 WO 6 nanosheets (BWO, 1.5 nm) were developed for photocatalytic degradation of ciprofloxacin. The samples with 5 % mass ratio of MS (5 %MS/BWO) exhibits the almost complete degradation of ciprofloxacin (≈100 %) under visible light. It is evidenced that the formation of S-scheme heterojunction with close interfacial interaction facilitates the photoinduced carrier separation and the generation of surface acid sites. The activation of ciprofloxacin molecules is realized through the coordinately interaction of C-N and C=O with the surface W sites. Moreover, the OVs in BWO side is a convenient pathway for activated of O 2 , embodying in the generation of •O 2 − and •OH under visible light over photocatalyst. Such an association of charge transfer mechanism with coordination activation shows the enhanced photocatalytic performance toward ciprofloxacin. This work provides a motivation which designs an S-scheme heterojunction photocatalyst with the ability to activate the specific group in molecules to comprehend the degradation of antibiotics.
研究领域:
材料科学
·
环境科学
·
化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Chaofan Zhang,Qiu Zhuang,Hao Wang,Xintong Ying,Ruoyang Ji,Daohu Sheng,Wei Dong,Aming Xie
Hexavalent chromium (VI) heavy metal contamination is considered a serious threat to human health and the environment. The photocatalytic reduction of Cr(VI) basically occurs in the acidic environment, severely limiting the application of photocatalysts for the reduction of Cr(VI). Therefore, we designed a microenvironment strategy to achieve efficient reduction of Cr (VI) under neutral conditions by introducing sulfonic acid onto the aromatic conjugated skeleton. A series of characterizations and experiments have shown that the sulfonated aromatic ring conjugated polymer (Arcp-SO 3 H) can efficiently remove Cr(VI) under neutral or even alkaline conditions. In neutral solutions, Arcp-SO 3 H has a rate constant of 0.054 min −1 within 90 min and has an efficiency of nearly 100 %, which is 16 times faster than before sulfonation (k = 0.0316 min −1 ). the Arcp-SO 3 H surpasses all organic polymers and most metal-based photocatalysts in the related field. The capture experiments have proved that •O 2 – is the main role of reducing Cr(VI), and e - is secondary, which is quite different from the mechanism reported in the previous literature. The efficiency of reducing Cr (VI) in the four-cycle experiment is still 96 %, which also proves that Arcp-SO 3 H has strong stability and reproducibility. Thus, Arcp-SO 3 H has great practical application potential in the treatment of wastewater, and microenvironmental strategies also offer new possibilities in the field of environmental remediation.
研究领域:
环境科学
·
材料科学
·
化学工程
·
水处理技术
·
光催化
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DOI
高影响因子
JOURNAL OF PHYSICS D-APPLIED PHYSICS
·
2024
·Vol. 57
·期 43
·435204
·
IF 3.1
Pengyu Zhao,Yikang Jia,Sihong Ma,Rui Zhang,Kaiyu Li,Tianyi Song,Jianbao Zheng,Jingyao Zhang,Li Guo,Dingxin Liu,Xiaohua Wang,Mingzhe Rong
Methicillin-resistant Staphylococcus aureus (MRSA) presents a significant threat due to the multiple resistance to antibiotics, leading to severe and challenging-to-treat infections. Plasma-activated saline (PAS) prepared by plasma gases, could efficiently inactivate various pathogenic bacteria including both sensitive and antibiotic-resistant bacteria. In this study, the PAS was prepared by plasma gases with different ratios of N2 and O2 activated by gliding arc discharge. First, the gaseous reactive species in the plasma gases were compared, revealing that the highest levels of NOx including NO2 and N2O5 were generated in the gases with the N2/O2 ratios of 4:6, 5:5, and 6:4. Subsequently, the PAS prepared by the two plasma-activated gases at the N2/O2 ratios of 5:5 and 6:4 exhibited the strongest inactivation effects on both planktic MRSA and biofilms. Furthermore, the aqueous reactive species in the PAS exhibited varied change trends with the increasing N2/O2 ratios. Additionally, ultraviolet spectroscopy combined with the probe of N, N-diethyl-p-phenylenediamine was applied for the detection of O2NOO− in the PAS, and the levels of O2NOO− in the PAS were positively correlated with the inactivation effects. Moreover, the PAS induced varying levels of nitration modification on the soluble proteins in MRSA cells, which were related to the intensities of O2NOO− in the PAS. This study regulated the reactive species in the PAS through gas composition and explored the inactivation mechanism of the PAS, providing a new strategy to promote the preparation efficiency of plasma-activated solutions for biomedical applications.
研究领域:
微生物学
·
生物医学工程
·
感染病学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zixian Qin,Yuxiu Sun,Zhengqing Zhang,Chenxu Zhang,Chi Tang,Chenxu Geng,Zhihua Qiao
Oxygen/nitrogen (O 2 /N 2 ) separation is of great importance but faces huge challenges owing to their similar molecular size and close polarity. In this work, we construct a polymer of intrinsic microporosity (PIM-1) based mixed matrix membrane (MMM) for efficient O 2 /N 2 separation by using ZIF-8 as the sieving filler along with surface modification of o-carborane (o-CB) to strengthen selective N 2 adsorption fixation as well as polymer-filler interfaces. Markedly, the o-CB on the outer surface of ZIF-8 not only affords the requisite interfacial compatibility in molecular sieving MMMs, but also increases the diffusion difference between O 2 and N 2 by the preferential adsorption with N 2 molecules. This synergistic effect of molecular sieving and adsorption inhibition achieves efficient O 2 /N 2 diffusion differential separation. As expected, the optimal membrane with o-CB-ZIF-8 loading of 35 wt% exhibits an O 2 permeability of 796.5 Barrer and a mixed O 2 /N 2 selectivity of 8.9 with O 2 /N 2 (20:80, vol.) mixtures, exceeding the latest 2015 upper bound limits. Moreover, the according membrane module with o-CB-ZIF-8 loading of 20 wt% also displays moderate O 2 permeability of 391.7 Barrer and O 2 /N 2 selectivity of 5.5 under pressure of 1 bar. This work may provide a feasible platform for designing high-performance MOF-based membranes in air separations.
研究领域:
材料科学
·
分离技术
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DOI
高影响因子
CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
·
2020
·
IF 0.936
Liang WANG,Zhang-Quan PENG
Development of lithium-oxygen (Li-O 2 ) batteries is hindered by large overpotentials, low energy efficiency and unsatisfactory cycling life, which are predominately caused by the oxygen evolution reaction (OER) involving sluggish oxidation of lithium peroxide (Li 2 O 2 ). Herein, a highly-efficient soluble redox mediator (RM) of N , N’ -Diphenyl- p -phenylenediamine (DPPD) is introduced to catalyze the oxygen evolution reaction for Li-O 2 batteries. During charging process, DPPD is electrochemically oxidized into DPPD + , which can chemically decompose Li 2 O 2 on the cathode with a much-reduced overpotential. The in-situ differential electrochemical mass spectrometry confirms that the charging process is dominated by Li 2 O 2 decomposition. With the assistance of DPPD, Li-O 2 cells can achieve lower charging potential, improved cycling stability, and prolonged lifespan (294 cycles) which is three times longer than that of tetrathiafulvalene counterpart. This work presents a credible and viable opportunity for long lifespan Li-O 2 batteries.
研究领域:
电化学
·
能源材料科学
✓ 已验证
DOI
高影响因子
NANOTECHNOLOGY
·
2019
·Vol. 30
·期 36
·364003
·
IF 3.399
Chao Li,Yijie Liu,Bojie Li,Fan Zhang,Zhu Cheng,Ping He,Haoshen Zhou
All-solid-state Li–O2 batteries are receiving intense interest because of the substitution of solid electrolytes for toxic and flammable liquid electrolytes. However, new issues are arising in the aspect of the electrolyte cathode interface. On the one hand, in a traditional sandwiched battery structure, the reaction sites of the cathode are restricted to the finite planar electrode–electrolyte interface, resulting in limited performance of all-solid-state Li–O2 batteries. On the other hand, integrating the electrolyte with the cathode to achieve good interfacial contact often requires complex sintering processes. Herein, this work reports a solid electrolyte cathode assembly (SECA) which consists of a dense Li1.5Al0.5Ge1.5P3O12 (LAGP) layer and a carbon coated porous LAGP layer fabricated by facilely one-step sintering. As a result, Li–O2 batteries adopting the SECA showed a relatively high discharge capacity of 0.48 mAh cm−2 at 5 μA cm−2. Besides, the batteries could sustain six full cycles with a restricted capacity of 0.08 mAh cm−2 at 10 μA cm−2. It was found that the high capacity can be attributed to the high surface area of porous cathode structure.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of Physical Chemistry C
·
2014
·
IF 4.835
Wugang Fan,Xiangxin Guo,Dongdong Xiao,Lin Gu
Gold nanoparticles (AuNPs) anchored to vertically aligned carbon nanotubes (VACNTs) act as additional nucleation sites for the Li2O2 growth, leading to the decreased size while increased density of Li2O2 particles in process of discharge. Correspondingly, at the deep discharge to 2.0 V the batteries show increased specific capacity. Upon charge, the AuNPs exhibit promotion effect on the Li2O2 decomposition by improving the conduction property of the discharge-formed particles, rather than by imposing the conventional electrocatalytic effect on the oxygen evolution reaction. Moreover, the AuNPs show promotion effect on decomposition of carbonate species arising from the side reactions. These effects consequently lead to the reduced charge overpotentials and extended cycle operation of the batteries. The results here provide a new as well as clear picture on the role of incorporated AuNPs in the Li2O2 formation and decomposition, which would be helpful for better understanding and constructing of high-performance air cathodes.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Binbin Shao,Yufan Chen,Deli Wu,Chaomeng Dai,Yalei Zhang
Structural Fe(II/III) hydroxides on the shell of nano-zerovalent iron (nZVI) are reactive sites for As(III) adsorption. Well-controlled structural Fe(II) hydroxides (SFH) is prepared to serve for As(III) removal in present study. With oxygen As(III) removal by SFH occurred efficiently but the removal efficiency was greatly reduced under anoxic conditions. The mineral transformation from SFH to lepidocrocite probably contributed to the robust removal efficiency of As(III). It is found that Cu(II), Cr(VI) and NO 2 − in aqueous solution could act as oxidants and promote the mineral transformation of SFH. A more efficient As(III) removal was therefore observed without oxygen. The removal efficiency decreased in the order O 2 /SFH ≈ Cu(II)/SFH > Cr(VI)/SFH ≈ NO 2 − /SFH at near neutral pH. The removal efficiency was less dependent on the initial pH for O 2 /SFH and Cu(II)/SFH systems than Cr(VI)/SFH and NO 2 − /SFH systems. Distribution of As on solid phases was able to describe the removal mechanism of As(III), and the results showed that the mineral transformation promoted the precipitation process and inhibited outer-sphere complexation, thus leading to enhanced As removal. With Cu(II), Cr(VI) and NO 2 − , the generation of oxidants from SFH transformation drove As(III) oxidation, and contributed to total As removal.
研究领域:
环境科学
·
化学
✓ 已验证
DOI
高影响因子
SusMat
·
2021
·Vol. 1
·期 3
·448-457
·
IF 0
Zhaomin Chen,Xiaoqing Gu,Yutong Guo,Xin Wang,Mingwang Shao,Bin Dong,Zhenhui Kang
Electrochemical cell can overcome the inherent intermittence of the renewable energy sources, thus showing great potentials in applications ranging from electrical energy storage to future smart grid. However, the current electrochemical cells could not achieve the “total green” feature by fully utilizing the clean and abundant O 2 /H 2 O redox couples due to the enormous overpotentials for both oxygen reduction reaction (ORR) and oxygen release reaction (OER). Herein, we report a “total green” electrochemical composite film cell based on carbon dots (CDots), which can realize both ORR and OER in the acid environment. The in-air voltage generation (0.95 V, with a maximum power of 5.3 μW) relies on the multiple-electron-transfer redox chemical reaction between the two active components inside the composite film, that is, ORR/OER of CDots and the redox reaction of polyaniline (PANI) on the electrode and the resulting proton concentration gradient. Interestingly, the cell can be self-recovered at low load, recharged by adding H 2 O 2 , or electrocharged at high load. We anticipate that current study may open up new opportunities for designing and developing total-green energy storage and conversion systems for diverse applications.
研究领域:
材料科学
·
能源技术
·
环境科学
✓ 已验证
DOI
JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Kang-Ning Gao,Hao-Ran Wang,Ming-Hui He,Yi-Qiu Li,Zhong-Hui Cui,Ya Mao,Tao Zhang
The development of solid-state lithium-oxygen batteries is currently limited primarily by the high solid-solid interfacial resistance and the lack of efficient assembly of electrolyte and electrode. In this work, noncovalent interactions between the cations of an ammonium ionic liquid and both solid electrolytes and carbon air cathodes are introduced. The ionic liquid-based electrolytes (ILE) are solidified on Li 6·40 La 3 Zr 1·40 Ta 0·60 O 12 (LLZTO) nanoparticles and gelated by multi-wall carbon nanotubes (MWCNTs), respectively, to construct LLZTO@ILE quasi-solid-state electrolyte (QSSE) and MWCNTs-LLZTO/ILE gel cathode (GC). The QSSE exhibits a high ionic conductivity of 1.71 × 10 −3 S cm −1 at 60 °C, high Li-ion transference number of 0.56, broad electrochemical window of ~4.8 V and good thermal stability . The GC shows outstanding compatibility with QSSE. Quasi-solid-state Li–O 2 batteries are assembled by integrating QSSE and GC films with a facile roll forming method, showing a low total interfacial resistance (~87 Ω cm 2 ), and excellent reversible cycles (70 cycles) with low charge overpotential (<0.44 V) and quite high electrical energy efficiency (>70%) at 60 °C and 200 mA g −1 . A 0.12 Ah pouch-type Li–O 2 battery was achieved by this method. These results suggest that the noncovalent interactions initiated by IL cations could be an effective approach to solve the solid-solid interface issue and achieve high discharge capacity in solid-state energy storage devices.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Xue Lu,Jingfang Li,Liye Liang,Guangming Li
Deep desulfurization with high-efficiency is imperia for environmental demands with increasing stringent standard of sulfur content in fuels. To develop high efficiency heterogeneous catalyst for aerobic oxidative desulfurization (AODS) of fuel, an Anderson-type CoMo 6 -2NH 2 (POM) as active site, which was considered to be very effective in catalyzing the activation of O 2 , was successfully anchored on the sub-stoichiometric ECOF as a carrier by Schiff-base condensation reaction between –NH 2 groups in CoMo 6 -2NH 2 and –CHO groups in ECOF. The anchoring of CoMo 6 -2NH 2 on ECOF by covalent bond resulted in the heterogenization of CoMo 6 -2NH 2 enabled CoMo 6 -2NH 2 @ECOF to be recyclable during the AODS process. When CoMo 6 -2NH 2 @ECOF was applied as catalyst for AODS of fuel with surfactant (OTAC) under O 2 , it exhibited excellent catalytic activity with almost 100 % removal rates under 95 °C for 6 h. Moreover, the catalyst can be recycled 7 times without significant loss of catalytic activity. Further, the structure-activity relationship was investigated and the reaction mechanism of AODS of fuel was verified by ESR, XPS analysis and selective quenching experiments.
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DOI
高影响因子
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