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Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution

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Journal of Energy Chemistry 2025年第1期100卷 226-233页

作者： Jingfang Zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang Key laboratory of Green Chemical engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Hubei Key Laboratory of Novel Reactor and Green Chemical Technology School of Chemical Engineering & Pharmacy Wuhan Institute of Technology Key laboratory of Pesticide & Chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education College of Chemistry Central China Normal University College of Materials Science and engineering Fuzhou University

Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction（OER）. Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER process. However, most of them undergo incomplete reconstruction with limited thickness of reconstruction layer, leading to low component utilization and arduous exploration of real catalytic mechanism. Herein, we identify the dynamic behaviors in complete reconstruction of Co-based complexes during OER. The hollow phytic acid（PA） cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability, in favor of the fast and complete reconstruction. A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co（Fe）(OH)xand subsequent potential-driven oxidation to Co（Fe）OOH. The obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm-2and a long-term *** experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER activity. The work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关键词： Complete reconstruction Co-based complex Precatalysts Oxygen evolution reaction

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Superhydrophobic and corrosion-resistant siloxane-modified MgAl-LDHs coatings on magnesium alloy prepared under mild conditions

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 450-463页

作者： Wenxi Zhang Zhangzelong Zhuo Dan Xu Liang Wu Zhihui Xie Chemical Synthesis and pollution control Key laboratory of Sichuan Province College of Chemistry and Chemical EngineeringChina West Normal UniversityNanchong 637002China College of Materials Science and engineering/National engineering Research Center for Magnesium Alloys Chongqing UniversityChongqing 400044China

We have developed a superhydrophobic and corrosion-resistant LDH-W/PFDTMS composite coating on the surface of Mg *** composite comprised a tungstate-intercalated(LDH-W)underlayer that was grown at low temperature(relative to hydrothermal reaction conditions)under atmospheric pressure and an outer polysiloxane layer created from a solution containing perfluorodecyltrimethoxysilane(PFDTMS)using a simple immersion *** successful intercalation of tungstate into the LDH phase and the following formation of the polysiloxane layer were confirmed through X-ray diffraction(XRD),Fourier transform infrared(FTIR)spectroscopy,and X-ray photoelectron spectroscopy(XPS).The corrosion resistance of the LDH-W film,both before and after the PFDTMS modification,was evaluated using electrochemical impedance spectroscopy(EIS),Tafel curves,and immersion *** results showed that Mg coated with LDH-W/PFDTMS exhibited significantly enhanced corrosion protection compared to the unmodified LDHW film,with no apparent signs of corrosion after exposure to 3.5wt%NaCl solution for 15 ***,the LDH-W/PFDTMS coating demonstrated superior superhydrophobicity and self-cleaning properties against water and several common beverages,as confirmed by static contact angle and water-repellency *** results offer valuable insights into preparing superhydrophobic and corrosion-resistant LDH-based composite coatings on Mg alloy surfaces under relatively mild reaction conditions.

关键词： Mg alloy corrosion coating layered double hydroxide

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Physical Layer Security Scheme With AoI-Awareness for Industrial IoT Based on Covert Communications

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IEEE/CAA Journal of Automatica Sinica 2025年第1期 276-278页

作者： Yaping Li Zhi-Xin Liu Jia-Wei Su Ya-Zhou Yuan the Key laboratory of Industrial Computer control engineering of Hebei Province Yanshan University

Dear Editor,Industrial Internet of things(IIoT) is a typical application of cyberphysical system(CPS). In the IIoT, wireless communication is an inevitable trend to replace the deployment-limited wired transmission for cases with large-scale and mobile devices. However, wireless communication gives rise to critical issues related to physical security, such as malicious detections and attacks [1].

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Removal of nitrogen from wastewater with perennial ryegrass/artificial aquatic mats biofilm combined system

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Journal of Environmental Sciences 2013年第4期25卷 670-676页

作者： Chongjun Chen Rui Zhang Liang Wang Weixiang Wu Yingxu Chen The Academy of water Science and Environmental engineering Zhejiang University Institute of Environmental Science and Technology Zhejiang University zhejiang provincial Key laboratory for water pollution control and Environmental Safety

To develop a cost-effective combined phytoremediation and biological process, a combined perennial ryegrass/artificial aquatic mat biofilm reactor was used to treat synthetic wastewater. Influent ammonium loading, reflux ratio, hydraulic retention time （HRT） and temperature all had significant effects on the treatment efficiency. The results indicated that the effluent concentration of ammonium increased with increasing influent ammonium loading. The reactor temperature played an important role in the nitrification process. The ammonium removal efficiency significantly decreased from 80% to 30%-50% when the reactor temperatttre dropped to below 10℃. In addition, the optimal nitrogen removal condition was a reflux ratio of 2. The nitrate and ammonium concentration of the effluent were consistent with the HRT of the combined system. The chemical oxygen demand （COD） removal efficiency was at a high level during the whole experiment, being almost 80% after the start-up, and then mostly above 90%. The direct uptake of N by the perennial ryegrass accounted for 18.17% of the total N removal by the whole system. The perennial ryegrass absorption was a significant contributor to nitrogen removal in the combined system. The result＇illustrated that the combined perennial ryegrass/artificial aquatic mat biofilm reactor demonstrated good performance in ammonium, total N and COD removal.

关键词： nitrogen perennial ryegrass biofilm wastewater treatment

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engineering atomic Rb-N configurations to tune radical pathways for highly selective photocatalytic H2O2 synthesis coupled with biomass valorization

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Journal of Energy Chemistry 2025年第1期100卷 215-225页

作者： Jiaye Li Shuang Pan Yihuang Chen Qiong Liu College of Chemistry and Materials engineering Wenzhou University Guangdong provincial Key laboratory of Chemical Measurement and Emergency Test Technology (China) Institute of Analysis Guangdong Academy of Sciences (China National Analytical CenterGuangzhou)

Photocatalytic oxygen reduction for hydrogen peroxide （H2O2） synthesis presents a green and costeffective production ***,achieving highly selective H2O2synthesis remains challenging,necessitating precise control over free radical reaction pathways and minimizing undesirable oxidative ***,we report for the visible light-driven simultaneous co-photocatalytic reduction of O2to H2O2and oxidation of biomass using the atomic rubidium-nitride modified carbon nitride（CNRb）.The optimized CNRb catalyst demonstrates a record photoreduction rate of 8.01 mM h-1for H2O2generation and photooxidation rate of 3.75 mM h-1for furfuryl alcohol to furoic acid,achieving a remarkable solar-to-chemical conversion （SCC） efficiency of up to 2.27%.Experimental characterizations and DFT calculation disclosed that the introducing atomic Rb–N configurations allows for the high-selective generation of superoxide radicals while suppressing hydroxyl free radical *** is because the Rb–N serves as the new alternative site to perceive a stronger connection position for O2adsorption and reinforce the capability to extract protons,thereby triggering a high selective redox product *** study holds great potential in precisely regulating reactive radical processes at the atomic level,thereby paving the way for efficient synthesis of H2O2coupled with biomass valorization.

关键词： Atomic economy Radical pathway regulation Rubidium atom coordination Biomass valorization

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Metal composition of layered double hydroxides(LDHs) regulating ClO_4^- adsorption to calcined LDHs via the memory effect and hydrogen bonding

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Journal of Environmental Sciences 2014年第3期26卷 493-501页

作者： Yajie Lin Qile Fang Baoliang Chen Department of Environmental Science Zhejiang University zhejiang provincial Key laboratory of Organic pollution Process and control

A series of calcined carbonate layered double hydroxides （CLDHs） with various metal compositions and different M^2＋/M^3＋ ratios were prepared as adsorbents for perchlorate. Adsorption isotherms fit Langmuir model well, and the adsorption amount followed the order of MgA1-CLDHs 1〉 MgFeCLDHs 〉〉 ZnA1-CLDHs. The isotherms of MgA1-CLDHs and MgFe-CLDHs displayed a two-step shape at low and high concentration ranges and increased with an increase in the M^2＋/M^3＋ ratio from 2 to 4. The two-step isotherm was not observed for ZnA1-CLDHs, and the adsorption was minimally affected by the M^2＋/M^3＋ ratio. The LDHs, CLDHs and the reconstructed samples were characterized by X-ray diffraction, SEM, FT-IR and Raman spectra to delineate the analysis of perchlorate adsorption mechanisms. The perchlorate adsorption of MgA1-CLDHs and MgFe-CLDHs was dominated by the structural memory effect and the hydrogen bonds between the free hydroxyl groups on the reconstructed-LDHs and the oxygen atoms of the perchlorates. For ZnAI-CLDHs, the perchlorate adsorption was controlled by the structural memory effect only, as the hydroxyl groups on the hydroxide layers preferred to form strong hydrogen bonds with carbonate over perchlorate, which locked the intercalated perchlorate into a more confined nano-interlayer. Several distinct binding mechanisms of perchlorate by CLDHs with unique M^2＋ ions were proposed.

关键词： calcined layered double hydroxidesperchlorateadsorption memory effecthydrogen bonds

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Tricrystalline TiO_2 with enhanced photocatalytic activity and durability for removing volatile organic compounds from indoor air

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Journal of Environmental Sciences 2015年第6期27卷 189-195页

作者： Kunyang Chen Lizhong Zhu Kun Yang Department of Environmental Science Zhejiang University zhejiang provincial Key laboratory of Organic pollution Process and control

It is important to develop efficient and economic techniques for removing volatile organic compounds（VOCs） in indoor air. Heterogeneous Ti O2-based semiconductors are a promising technology for achieving this goal. Anatase/brookite/rutile tricrystalline Ti O2 with mesoporous structure was synthesized by a low-temperature hydrothermal route in the presence of *** obtained samples were characterized by X-ray diffraction and N2 adsorption-desorption isotherm. The photocatalytic activity was evaluated by photocatalytic decomposition of toluene in air under UV light illumination. The results show that tricrystalline Ti O2 exhibited higher photocatalytic activity and durability toward gaseous toluene than bicrystalline Ti O2,due to the synergistic effects of high surface area, uniform mesoporous structure and junctions among mixed phases. The tricrystalline Ti O2 prepared at R HNO3= 0.8, containing80.7% anatase, 15.6% brookite and 3.7% rutile, exhibited the highest photocatalytic activity,about 3.85-fold higher than that of P25. The high activity did not significantly degrade even after five reuse cycles. In conclusion, it is expected that our study regarding gas-phase degradation of toluene over tricrystalline Ti O2 will enrich the chemistry of the Ti O2-based materials as photocatalysts for environmental remediation and stimulate further research interest on this intriguing topic.

关键词： VOC Photocatalysis Tricrystalline TiO2 Nanomaterials Mesoporous Gaseous

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Enhancing plant-microbe associated bioremediation of phenanthrene and pyrene contaminated soil by SDBS-Tween 80 mixed surfactants

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Journal of Environmental Sciences 2014年第5期26卷 1071-1079页

作者： Hewei Ni Wenjun Zhou Lizhong Zhu Department of Environmental Science Zhejiang University zhejiang provincial Key laboratory of Organic pollution Process and control

The use of surfactants to enhance plant-microbe associated dissipation in soils contaminated with polycyclic aromatic hydrocarbons （PAHs） is a promising bioremediation technology. This comparative study was conducted on the effects of plant-microbe treatment on the removal of phenanthrene and pyrene from contaminated soil, in the presence of low concentration single anionic, nonionic and anionic-nonionic mixed surfactants. Sodium dodecyl benzene sulfonate （SDBS） and Tween 80 were chosen as representative anionic and nonionic surfactants, respectively. We found that mixed surfactants with concentrations less than 150 mg/kg were more effective in promoting plant-microbe associated bioremediation than the same amount of single surfactants. Only about （m/m） of mixed surfactants was needed to remove the same amount of phenanthrene and pyrene from either the planted or unplanted soils, when compared to Tween 80. Mixed surfactants （〈 150 mg/kg） better enhanced the degradation efficiency of phenanthrene and pyrene via microbe or plant-microbe routes in the soils. In the concentration range of 60-150 mg/kg, both ryegrass roots and shoots could accumulate 2-3 times the phenanthrene and pyrene with mixed surfactants than with Tween 80. These results may be explained by the lower sorption loss and reduced inteffacial tension of mixed surfactants relative to Tween 80, which enhanced the bioavailability of PAHs in soil and the microbial degradation efficiency. The higher remediation efficiency of low dosage SDBS-Tween 80 mixed surfactants thus advanced the technology of surfactant-enhanced plant-microbe associated bioremediation.

关键词： polycyclic aromatic hydrocarbons contaminated soil plant-microbe associated bioremediation ryegrass

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Acid-assisted hydrothermal synthesis of nanocrystalline TiO_2 from titanate nanotubes: Influence of acids on the photodegradation of gaseous toluene

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Journal of Environmental Sciences 2015年第1期27卷 232-240页

作者： Kunyang Chen Lizhong Zhu Kun Yang Department of Environmental Science Zhejiang University zhejiang provincial Key laboratory of Organic pollution Process and control

In order to efficiently remove volatile organic compounds（VOCs） from indoor air, onedimensional titanate nanotubes（Ti NTs） were hydrothermally treated to prepare TiO2 nanocrystals with different crystalline phases, shapes and sizes. The influences of various acids such as CH3 COOH, HNO3, HCl, HF and H2SO4 used in the treatment were separately compared to optimize the performance of the TiO2 nanocrystals. Compared with the strong and corrosive inorganic acids, CH3COOH was not only safer and more environmentally friendly, but also more efficient in promoting the photocatalytic activity of the obtained TiO2. It was observed that the anatase TiO2 synthesized in 15 mol/L CH3COOH solution exhibited the highest photodegradation rate of gaseous toluene（94%）, exceeding that of P25（44%） by a factor of more than two. The improved photocatalytic activity was attributed to the small crystallite size and surface modification by CH3COOH. The influence of relative humidity（20%–80%） on the performance of TiO2 nanocrystals was also studied. The anatase TiO2 synthesized in 15 mol/L CH3COOH solution was more tolerant to moisture than the other TiO2 nanocrystals and P25.

关键词： Titanate nanotubes CH3COOH Ti O2nanocrystals Photocatalytic Gaseous toluene

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Performance of bimetallic nanoscale zero-valent iron particles for removal of oxytetracycline

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Journal of Environmental Sciences 2018年第7期30卷 173-182页

作者： Yuwei Wu Qinyan Yue Yuan Gao Zhongfei Ren Baoyu Gao Shandong provincial Key laboratory of water pollution control and Resource Reuse School of Environmental Science and EngineeringShandong University

In this study, bimetallic nanoscale zero-valent iron particles（nZVI）, including copper/nanoscale zero-valent iron particles（Cu/nZVI） and nickel/nanoscale zero-valent iron particles（Ni/nZVI）, were synthesized by one-step liquid-phase reduction and applied for oxytetracycline（OTC） removal. The effects of contact time and initial p H on the removal efficiency were studied. The as-prepared nanoscale particles were characterized by scanning electron microscopy（SEM）, energy dispersive spectroscopy（EDS） and X-ray diffraction（XRD）. Finally, the degradation mechanisms of OTC utilizing the as-prepared nanoparticles were investigated by using X-ray photoelectron spectroscopy（XPS） and mass spectrometry（MS）. Cu/n ZVI presented remarkable ability for OTC degradation and removed71.44% of OTC（100 mg/L） in 4 hr, while only 62.34% and 31.05% of OTC was degraded by Ni/nZVI and nZVI respectively. XPS and MS analysis suggested that OTC was broken down to form small molecules by ·OH radicals generated from the corrosion of Fe0. Cu/nZVI and Ni/n ZVI have been proved to have potential as materials for application in OTC removal because of their significant degradation ability toward OTC.

关键词： Bimetallic nanoscale zero-valent iron particles Oxytetracycline Degradation mechanism Hydroxyl radicals

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