CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xiangcheng Zhang,Jingzhen Zhang,Jie Miao,Xue Wen,Chao Chen,Baoxue Zhou,Mingce Long
Photocatalytic H 2 O 2 production is a promising strategy for decentralized applications, but to realize efficient H 2 O 2 production in the ambient conditions and absence of organic sacrifice remains challengeable. Herein, anthraquinone functionalized covalent organic frameworks (TpAQ-COFs) were fabricated by β-ketoenamines links of 2,6-diaminoanthraquinone (AQ) and 2, 4, 6-triformylphloroglucinol (Tp), and the structures and compositions were tuned by controlling the condensation time. The increase of time favors the assembly of TpAQ-COFs into more ordered lamellar stacking structure, and induces the increase of enol-imine form. The critical role of anthraquinone moieties as the active sites for oxygen reduction was proved, that is, facilitating charge separation and enhancing the activity and selectivity of H 2 O 2 production. Upon visible light irradiation, the TpAQ-COF synthesized after 12 h reaction has the highest content of anthraquinone moieties and the best performance for H 2 O 2 production (420 μmol h −1 g −1 ) in the absence of organic sacrificial agents. These findings bring insights to incorporate anthraquinone chemistry into photocatalysts at molecular levels for efficient H 2 O 2 production.
研究领域:
材料科学
·
环境科学
·
化学
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产品关联
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
✓ 已验证
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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产品关联
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
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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
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
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
Nano Research
·
2018
·Vol. 12
·期 3
·517-523
·
IF 7.994
Liu Tie,Wang Leidanyang,Huang Tao,Yu Aishui
Design and fabrication of framework-structured porous precursors have been regarded as a prospective albeit challenging strategy to obtain bimetal/NC-enriched bifunctional elecrocatalysts. In this work, an effective bottom-up approach involving solution-based self-assembly and a post-annealing process was developed to confine (Co, Zn)-N-C active sites into N-enriched graphitic carbon nanocages. This novel architecture containing N-doped-C stabilized bimetallic nanoparticles derived from ZIF precursors was well-studied by a series of characterization and analysis techniques. Details were given that these well-dispersed (Co, Zn) nanoparticles were encapsulated into the pyridinic-N-dominated graphitic carbon nanocage with a total metal loading of approximately 7.4 at.%. This favorable hierarchical structure not only enhances the electron conductivity, but also owns a sufficient BET surface area facilitating the gas-liquid-solid triphase reaction and producing more space to store discharge products. Importantly, results infer that the interesting nanoframes manifests a satisfying ORR/OER activity and enhanced cell performance whether liquid or solid-state electrolytes are used. As such, our work rationalizes that this type of cage-shaped bimetal-N-C material is promising for high-performance Li-O 2 batteries.
研究领域:
材料科学
·
电化学
·
纳米催化
·
能源存储
·
功能材料
✓ 已验证
DOI
高影响因子
Science China-Materials
·
2016
·Vol. 59
·期 8
·618-628
·
IF 0
Yi Ting-Feng,Han Xiao,Yang Shuang-Yuan,Zhu Yan-Rong
Layered Li 1.2 Mn 0.56 Ni 0.16 Co 0.08− x
Al
x
O 2 (0 ≤ x ≤ 0.08) cathode materials were successfully synthesized by a sol-gel method. X-ray diffraction and the refinement data indicate that all materials have typical α-NaFeO 2 structure with R -3 m space group, and the a -axis has almost no change, but there is a slight decrease in the c lattice parameter as well as the cell volume. Scanning electron microscopy and high resolution transmission electron microscopy prove that all the samples have uniform particle size of about 200–300 nm and smooth surface. The energy-dispersive X-ray spectroscopy mapping shows that aluminum has been homogeneously doped in the Li 1.2 Mn 0.56 Ni 0.16 Co 0.08 O 2 cathode material. The cyclic voltammetry and electrochemical impedance spectroscopy reveal that appropriate Al-doping contributes to the reversible lithium-ion insertion and extraction, and then reduces the electrochemical polarization and charge transfer resistance. Li 1.2 Mn 0.56 Ni 0.16 Co 0.08− x
Al
x
O 2 ( x = 0.05) shows the lowest charge transfer resistance and the highest lithium-ion diffusion coefficient among all the samples. The Li-rich electrodes with low-level Al doping shows a much higher discharge capacity than the pristine one, especially the Li 1.2 Mn 0.56 Ni 0.16 Co 0.08− x
Al
x
O 2 ( x = 0.05) sample, which exhibits greater rate capacity and better fast charge-discharge performance than the other samples. Li 1.2 Mn 0.56 Ni 0.16 Co 0.08− x
Al
x
O 2 ( x = 0.05) also exhibits higher discharge capacity than the pristine one at each cycle at 55°C. These results clearly indicate that the high rate capacity together with a good high rate cycling performance and high-temperature performance of the low-Co Li 1.2 Mn 0.56 Ni 0.16 Co 0.08− x
Al
x
O 2 ( x =0.05) is a promising alternative to next-generation lithium-ion batteries.
研究领域:
材料科学
·
电化学
·
储能技术
·
锂离子电池
✓ 已验证
DOI
PROCEEDINGS OF THE COMBUSTION INSTITUTE
·
2020
·Vol. 38
·期 4
·5475-5484
·
IF 5.627
Jianghui Luo,Qianjin Lin,Wenxiang Xia,Yizhuo He,Mei Mei,Lixin Lu,Yang Liu,Chun Zou
Pressurized oxy-fuel combustion has been attracting increasing attentions due to its improved efficiency and low cost. The present study reports ignition delay times (IDTs) of pyridine under O 2 /CO 2 atmospheres within a temperature range from 1202 to 1498 K at pressures from 2.2 to 10 bar for equivalence ratios of 0.5, 1.0, and 2.0. The experimental results were compared with the IDTs of pyridine under O 2 /Ar atmospheres from MacNamara et al.. The comparison results indicate that the IDTs of pyridine under O 2 /CO 2 atmospheres are evident longer than those under O 2 /Ar atmospheres even at low pressure. A modified kinetic model (HUST pyridine Model) was proposed based on our previous mechanism. HUST pyridine Model predicted well the IDTs under both O 2 /CO 2 and O 2 /Ar atmospheres obtained in shock tubes and the species profiles under both O 2 /CO 2 and O 2 /N 2 atmospheres obtained in plug flow reactors . HUST pyridine Model, Alzueta Model, and Pyridine LTO Model were evaluated. The results show that the performance of HUST pyridine Model is much better than Alzueta Model, and Pyridine LTO Model. The main reason is that the net reaction rate of C 5 H 5 N + O = C 5 H 4 N + OH in HUST pyridine Model is much faster than that in Aluzeta Model. The effect of CO 2 on the ignition of pyridine at elevated pressures has been analyzed in detail. The oxidation pathways of pyridine are also analyzed at different pressures.
研究领域:
燃烧化学
·
化学动力学
·
能源工程
·
燃料科学
·
高压物理
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 2
·740-751
·
IF 12.732
Lichong Peng,Yaxin Sun,Shiquan Guo,Congju Li
Oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) involve proton coupled electron transfer reaction (PCET), resulting in sluggish redox kinetics. At present, the development of high-efficiency bifunctional oxygen electrocatalysts is still a puzzling challenge. Herein, we propose a scalable strategy for embedding and beading ZIF-derived hollow Co–Nx nanocube cage dispersion implanted with porous carbonized nanofibers (EH/PCNFs and BH/PCNFs) through electrospinning and annealing. The cobalt species prevent themselves from agglomerating during the annealing process through the “fence” effect of the non-volatile Zn species, thereby synergizing with ligand volatilization to facilitate the formation of Co–Nx nanocube cages. Benefiting from the ultralong interconnected multi-layered carbon nanofiber matrix, the hollow Co–Nx nanocube cages can change the charge density and electron distribution of the carbon nanofiber matrix, endowing the carbonized nanofiber carrier with special surface polarization and accelerating the electrocatalytic kinetics. Remarkably, the integrated Li–O2 batteries (LOBs) based on BH/PCNFs and EH/PCNFs electrodes exhibit significantly decreased charge/discharge polarization (0.79 V) and a long-term cyclability (147 cycles) under a cut off capacity of 500 mA h g−1 at 200 mA g−1. This work might be beneficial for the practically viable design and manufacture of dual-function oxygen electrocatalysts.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
JOURNAL OF POLYMER SCIENCE
·
2026
·
IF 3.9
Jialong Yang,Guangqun Zhai
The effect of H 2 O 2 and H 2 O 2 -ascorbic acid (Vc) pairs on defunctionalization of 2-cyano-2-propyl dithiobenzoate (CPDB) and CPDB-mediated reversible addition-fragmentation chain transfer (RAFT) polymerization of methyl methacrylate (MMA) in dimethyl sulfoxide (DMSO) is investigated. The stability of CPDB toward H 2 O 2 is monitored by UV–vis absorption spectroscopy. CPDB is partially defunctionalized by H 2 O 2 alone and more seriously by H 2 O 2 -Vc pairs at 40°C, due to the oxidation by H 2 O 2 and the stepwise addition of DMSO-derived H 3 C· radicals. MMA greatly inhibits the defunctionalization of dithiobenzoate moieties, as both HO· and H 3 C· radicals incur oligomeric MMA-terminated alkyl radicals, which conserve the dithiobenzoate moieties of CPDB. H 2 O 2 -Vc-initiated CPDB-mediated RAFT polymerization is undertaken at 30°C and 40°C. Conversion is measured by gas chromatography, and molecular weight (MW) of PMMA is determined by gel-permeation chromatography. The processes manifest a moderately controlled fashion under optimal conditions. The products at low conversion display a multi-component composition, with high-MW PMMA consisting of 90% at least. MW of PMMA increases almost linearly with the yield and maintains a narrow distribution, but higher than the corresponding theoretical MW, owing to the partial defunctionalization of CPDB. Mass spectroscopy reveals that the irreversible termination of the intermediate radicals is the primary factor. Graphical H 2 O 2 initiated reversible addition-fragmentation chain transfer (RAFT) polymerization in dimethyl sulfoxide (DMSO) with 2-cyano-2-propyl dithiobenzoate (CPDB) as both the reducing agent and CTA. The defunctionalization of CPDB by H 2 O 2 in DMSO was observed, but methyl methacrylate significantly inhibited the defunctionalization. The CPDB-mediated RAFT polymerization was fulfilled with H 2 O 2 or H 2 O 2 -Vc pairs as the initiator. MS attributed the defunctionalization to the formation and the irreversible termination of lower-activity intermediate radicals.
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产品关联
DOI
高影响因子
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