CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Ruxin Peng,Jihai Shao,Yuanlin Xie,Anwei Chen,Liang Peng,Qingru Zeng,Si Luo
Being that the influence of organic ligands on contaminant removal by nanoscale zero valent iron (nZVI) has been explored in quite a few studies, there is little information on reaction mechanisms of the ZVI-ligand system under different aeration conditions. The degradation of nitrobenzene (NB) by nZVI-oxalic acids (OA) was investigated under N 2 , O 2 and without aeration conditions. From the findings, it was evident that OA dramatically improved NB degradation by nZVI with all of the aeration conditions. Approximately 100% of NB was degraded by nZVI-OA+N 2 system after 60 min of reaction, followed in effectiveness by nZVI-OA+ without aeration (95%) as well as nZVI-OA+O 2 (85%). Operation parameters including OA concentration and pH had significant effect on the removal of NB in the nZVI-OA system. 3 mM OA concentration and pH 3.0 were found to be favourable. The Fe 2+ , total dissolved iron concentrations, pH and ORP values in the nZVI-OA systems had also been monitored. Intermediates and trapping experiments showed that reduction played a fundamental role in the NB degradation by nZVI-OA under N 2 or without aeration conditions. The formation of Fe(OA) 0 and Fe(OA) 2 2− complexes had lower standard ORP, which could improve the strength of reductant in the systems, and thus resulting in an increased degradation efficiency of NB by nZVI-OA+N 2 . Under O 2 aeration condition, the NB degradation process could be regarded as an oxidation . In the meantime, OA promoted the production of reactive oxidants species by speeding up the oxidation rates of Fe 2+ by O 2 and H 2 O 2 . Summarily, the improved reactivity of nZVI was largely as a result of the strong complexation ability of OA.
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2017
·Vol. 164
·期 13
·G112
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IF 3.259
Yuchen Hui,Xiaoyan Ma,Fengjin Qu,Fang Chen,Ying Chen
A practical strategy is developed to fabricate stable glucose/O2 biofuel cells with high power density assembled by enzymatic bio-electrodes based on three-dimensional nickel foam. The porous three-dimensional nickel foam is used as a substrate to enhance the enzyme loading, while the reduced graphene oxide and gold nanoparticles decorating on the nickel foam are employed as the direct electron transfer system for bio-anodes and bio-cathodes. The ferrocenecarboxylic acid serves for the mediated electron transfer to further increase electron transfer rate for glucose oxidase electrodes. Covalent bond is employed to immobilize the mediator and enzymes for improving the stability of bio-electrodes and biofuel cells. As the results, the surface glucose oxidase loading reaches to 4.03 × 10−7 mol cm−2 with good enzymatic activity. Additionally, the obtained glucose/O2 biofuel cells exhibit an outstanding maximum power density of 2.84 ± 0.09 mW cm−2, with a remarkable long-term operational stability for retaining 85.5% of its performance after 70 days. In human blood, the biofuel cell shows a favorable output performance of 0.39 ± 0.04 mW cm−2, implying the appropriateness for practical applications.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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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
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材料科学
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化学工程
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水处理技术
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光催化
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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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
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环境科学
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化学
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高影响因子
ACS Catalysis
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2025
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IF 13.1
Weina Yang,Yachao Wang,Yaxiong Wei,Guofeng Zhao,Weixin Huang,Cong Fu
Photocatalytic oxidative coupling of methane (OCM) offers a sustainable pathway for direct conversion of methane into value-added hydrocarbons, yet faces persistent challenges in balancing efficient methane activation with suppression of overoxidation. Here, we present a TiO2-based photocatalyst decorated with highly dispersed Ag–Co dual sites that achieves superior performance in continuous-flow OCM. The optimized AgCo–TiO2 system demonstrates a remarkable C2 hydrocarbon production rate of 1.7 mmol g–1 h–1 with 91% selectivity while maintaining stable operation for over 30 h. In situ spectroscopic analyses indicate that the introduced Co species induce mobile-charge imbalances, driving the directional transfer of photogenerated electrons and effectively suppressing electron–hole recombination. Coupled with Ag serving as a catalytic center, these effects synergistically enhance O2 activation, C–H bond cleavage, and selective C–C coupling, thereby contributing to the superior catalytic performance. This work provides valuable mechanistic insights into the photocatalytic OCM process, highlighting the pivotal role of precisely engineered charge transfer pathways in enabling efficient methane-to-C2 conversion.
研究领域:
光催化
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材料科学
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化学工程
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环境化学
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能量转换
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Hao Jiang,Mei Yan,Hao Chen,Yutuo Fu,Chongshen Guo
Strong Coulomb force between photogenerated electrons and holes often results in high level exciton pairs during the photocatalytic process, which hinders the formation of reactive oxygen species (ROS) in the photocatalytic reaction, particularly for the photocatalysis under near infrared (NIR) irradiation. Hence, it is crucial to dissociate excitons into free carriers. In this study, we propose a novel amorphous–crystalline heterojunction of a-CeO 2 /SnFe 2 O 4 for the NIR-driven photocatalytic degradation and sterilization. The introduction of disorder–order interface in heterojunction could greatly enhance the built-in electric field, thereby serving for exciton dissociation. Additionally, the presence of oxygen vacant sites in the a-CeO 2 /SnFe 2 O 4 system can effectively modulate the electronic structure of the material, facilitating exciton dissociation in conjunction with the built-in electric field. The DFT simulation proved the positive impact of the disorder–order interface on charge separation, as well as its enhancement on the activation of O 2 and H 2 O molecules. This work provides a theoretical support for the creation of disorder–order interface to promote exciton dissociation and enhance photocatalytic performance.
研究领域:
材料科学
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光催化
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表面化学
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理论化学
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高影响因子
Journal of Environmental Chemical Engineering
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2025
·Vol. 13
·期 6
·120354
·
IF 7.2
Dan Dang,Xinyi Jiang,Juncheng Zhang,Yichao Wu,Baoxin Zha,Yingying Zhao
The valorization of crude glycerol, a major byproduct of biodiesel production, into high-value chemicals is critical for sustainable biorefineries. Herein, we report a novel alkali-free and homogeneous photocatalytic strategy for selectively converting glycerol to glycolic acid (GLYA) and formic acid (FA) using H 2 O 2 as a radical initiator under 365 nm UV irradiation. By optimizing volume fraction of H 2 O 2 (3.18％), light intensity (10 W), and temperature (35 °C), 99.3 % glycerol conversion with 23.47 % GLYA yield and 22.66 % FA yield was achieved within 2 h at ambient pressure. Crucially, scavenging experiments, post-illumination reactivity studies and the electron paramagnetic resonance (EPR) spectra revealed a synergistic •OH /•O 2 ⁻/ 1 O 2 radical cycle triggered by H 2 O 2 photolysis: (1) •OH initiates glycerol oxidation to glyceraldehyde; (2) •O 2 ⁻ (generated from O 2 reduction or H 2 O 2 decomposition) produces 1 O 2, which drives selective C-C cleavage to GLYA; (3) •OH/•O 2 ⁻/ 1 O 2 cycle enables mutual regeneration of active species, sustaining oxidation even after light cessation. This autocatalytic cycle eliminates the need for strong bases or noble metals, offering a green, energy-efficient route for glycerol upcycling.
研究领域:
催化化学
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绿色化学
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可再生能源
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环境科学
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化学工程
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高影响因子
ACS Applied Materials & Interfaces
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2023
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IF 9.5
Zaiyong Yang,Zhiheng Hao,Shunxin Zhou,Peng Xie,Zengxi Wei,Shuangliang Zhao,Fuzhong Gong
Direct synthesis of hydrogen peroxide (DSHP) from H2 and O2 offers a promising alternative to the present commercial anthraquinone method, but it still faces the challenges of low H2O2 productivity, low stability of catalysts, and high risk of explosion. Herein, by loading in a microchannel reactor, the as-synthesized Pd–Sn alloy materials exhibit high catalytic activity for H2O2 production, presenting a H2O2 productivity of 3124 g kgPd–1 h–1. The doped Sn atoms on the surface of Pd not only facilitate the release of H2O2 but also effectively slow down the deactivation of catalysts. Theoretical calculations demonstrate that the Pd–Sn alloy surface has the property of antihydrogen poisoning, showing higher activity and stability than pure Pd catalysts. The deactivation mechanism of the catalyst was elucidated, and the online reactivation method was developed. In addition, we show that the long-life Pd–Sn alloy catalyst can be achieved by supplying an intermittent flow of hydrogen gas. This work provides guidance on how to prepare high performance and stable Pd–Sn alloy catalysts for the continuous and direct synthesis of H2O2.
研究领域:
化学工程
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催化科学
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材料科学
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2021
·Vol. 46
·期 3
·2737-2747
·
IF 5.164
Yueheng Fan,Aiming Wu,Xiaohui Yan,Shuiyun Shen,Zhang Junliang
Summary Both the activity and structure of a cathode, when it is used in non-aqueous Li-O 2 batteries, play a prominent role in the aspects of durability and capacity. In this work, α-MnO 2 /prGO hybrid nanocomposites with a three-dimensional (3D) porous structure are proposed to act as the cathode to improve the battery performance. Highly active α-MnO 2 /prGO nanocomposites with different mass ratios are synthesized through a two-step template method and a subsequent annealing process. It is found that the optimal 50% α-MnO 2 /prGO cathode exhibits outstanding discharge capacity of 13 294 mAh g −1 under the condition of 100 mA g −1 . Meanwhile, with the limited capacity and currency density of 1000 and 100 mA g −1 , respectively, the battery maintains excellent durability for 239 cycles. Significantly, it is clear that the excellent electrochemical performance of the nanocomposites is strongly associated with the synergistic effect of their distinct porous architecture and the ORR/OER catalytic activity.
研究领域:
材料科学
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电化学
·
能源存储与转换
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高影响因子
Journal of the American Chemical Society
·
2014
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IF 11.444
Xibin Pang,Wei Chang,Chuncheng Chen,Hongwei Ji,Wanhong Ma,Jincai Zhao
The molecules O2 and H2O dominate the cleavage of aromatic sp2 C–C bonds, a crucial step in the degradation of aromatic pollutants in aqueous TiO2 photocatalysis, but their precise roles in this process have remained elusive. This can be attributed to the complex oxidative species involved and to a lack of available models for reactions with a high yield of direct products. Here, we used oxygen-18 isotope labeled O2 and H2O to observe the aromatic ring-opening reaction of the model compound 3,5-di-tert-butylcatechol (DTBC), which was mediated by TiO2 photocatalysis in an aqueous acetonitrile solution. By analyzing the primary intermediate products (∼75% yield), especially the seven-membered ring anhydrides that were formed, we obtained direct evidence for the oxygen atom of dioxygen insertion into a C–C bond of the aromatic ring. This indicates that molecular oxygen is the ultimate ring-opening agent in TiO2 photocatalysis and that it undergoes single O atom incorporation rather than the previously proposed molecular oxygen 1,2-addition processes. The ratio of intradiol to extradiol products depends on the particle size of TiO2 catalysts used, which suggests that the O2 activation is correlated with the available coordination sites on the TiO2 surface in the photocatalytic cleavage of the aromatic ring.
研究领域:
环境科学
·
化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Shumin Li,Jun Tan,Zhejun Jiang,Jin Wang,Zhengquan Li
Dye-sensitized systems show promising in photocatalysis because they can separate the tasks of light absorption, charge generation and surface catalysis to two coupled components. In this system, it is crucial to develop suitable catalysts capable of receiving dye-injected charges and having high activity to a given reaction. Aiming to photocatalytic H 2 and O 2 production, we present a metal-organic framework derived route to prepare bimetallic Fe-Ni-P nanotubes using Fe-Ni-MIL-88 nanorods as templates. When integrated with different dyes, these Fe-Ni-P nanotubes can serve as efficient catalysts for photocatalytic H 2 and O 2 production, respectively. Additionally, catalytic activities of such dye-sensitized systems can be conveniently regulated by tailoring the metal compositions in Fe-Ni-P nanotubes. The photocatalytic H 2 production of Fe 1 -Ni 2 -P can reach 5420 μmol g cat −1 h −1 under eosin-Y sensitization, which is 24 times and 6.7 times higher than Fe 2 P and Ni 2 P, respectively. The photocatalytic O 2 production of Fe 1 -Ni 2 -P can reach 900.3 μmol g cat −1 h −1 under [Ru(bpy) 3 ]Cl 2 sensitization, about 4.6 times and 2.9 times higher than Fe 2 P and Ni 2 P. The roles of different components in the system have been explored and corresponding working mechanism is proposed. This work demonstrates a new type of dye-sensitized systems consisting of bimetallic phosphides and provides a facile route to regulate their photocatalytic performance.
研究领域:
材料科学
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光催化
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高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 25
·10008-10013
·
IF 8.262
Jin-ling Ma,Xin-bo Zhang
Development of an efficient air cathode for metal–air batteries composed of an element that is abundant on earth is a scientific and technical challenge. Here, nitrogen (N)-doped carbon cathodes were prepared using two conventional doping methods, namely ammonia activation (ammoxidation) and introduction of an N-containing precursor. Interestingly, the introduction of N-containing precursors to prepare the N-doped carbon material not only gave a different pore distribution with increased surface area but also maintained considerable N content, unlike the use of the ammoxidation method – thus greatly enhancing the catalytic activity (low overpotential) and improving the discharge capacity (6905 mA h g−1) and cycle life (from 8 to 66 cycles) in sodium–oxygen batteries compared with the pure carbon material. This study also stresses the importance of adopting the optimized synthesis method to prepare the N-doped carbon cathode.
研究领域:
电化学
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能源材料
·
纳米材料
·
电池技术
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多孔材料科学
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高影响因子
危险品化学品经营许可证（带存储）