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Electrocoagulation coupled with Electrooxidation for the simultaneous treatment of multiple pollutants in contaminated sediments

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Journal of Environmental Sciences 2023年第2期124卷 89-97页

作者： Qingjun Zeng Yifan Zhang Pingshan Chen Yuting He Congli Yi Chunhua Feng Fourth Harbor Engineering Institute Co. Ltd.China Communications Construction Co.Ltd.Guangzhou 510230China Key Laboratory of Environmental Protection&Safety of Communication Foundation Engineering China Communications Construction Co.Ltd.Guangzhou 510230China The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationSchool of Environment and EnergySouth China University of TechnologyGuangzhou 510006China

In situ and simultaneous remediation of a variety of pollutants in sediments remains a challenge.In this study,we report that the combination of electrocoagulation(EC)and Electrooxidation(EO)is efficient in the immobilization of phosphorus and heavymetals and in the oxidation of ammonium and toxic organicmatter.The integratedmixed metal oxide(MMO)/Fe anode system allowed the facile removal of ammonium and phosphorus in the overlying water(99% of 10 mg/L NH_(4)^(+)-N and 95% of 10 mg/L P disappeared in 15 and 30 min,respectively).Compared with the controls of the single Fe anode and single MMO anode systems,the dual MMO/Fe anode system significantly improved the removal of phenanthrene and promoted the transition of Pb and Cu from the mobile species to the immobile species.The concentrations of Pb and Cu in the toxicity characteristic leaching procedure extracts were reduced by 99%and 97% after an 8 hr operation.Further tests with four real polluted samples indicated that substantial proportions of acid-soluble fraction Pb and Cu were reduced(30%-31% for Pb and 16%–23% for Cu),and the amounts of total organic carbon and NH_(4)^(+)-N decreased by 56%–71% and 32%–63%,respectively.It was proposed that the in situ electrogenerated Fe(II)at the Fe anode and the active oxygen/chlorine species at the MMO anode are conducive to outstanding performance in the co-treatment of multiple pollutants.The results suggest that the EC/EO method is a powerful technology for the in situ remediation of sediments contaminated with different pollutants.

关键词： In situ sediment remediation Electrocoagulation Electrooxidation Stabilization of heavy metals Ammonia oxidation Removal of polycyclic aromatic hydrocarbons

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Atomic engineering promoted Electrooxidation kinetics of manganese-based cathode for stable aqueous zinc-ion batteries

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Nano Research 2022年第9期15卷 8603-8612页

作者： Hao Luo Lipeng Wang Penghui Ren Jiahuang Jian Xiong Liu Chaojiang Niu Dongliang Chao School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China Laboratory of Advanced Materials Fudan UniversityShanghai 200433China MHT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China

Rechargeable zinc-based batteries with near-neutral media are standing in the middle of the energy storage field by virtue of their high safety and low cost.However,it is still imperative for Mn-based cathode to improve rate capacity by facilitating ions/electron transfer and long-cycle stability by suppressing Mn dissolution.Herein,promoting Electrooxidation kinetics is proposed and employed to construct advanced Mn-Zn battery.The formation of carbon-protected birnessite-MnO_(2)is promoted via inducing the electron-donating capability of the heterointerface between the N-C coating and the defective MnO.Moreover,density functional theory calculations also demonstrate that N-C protected birnessite-MnO_(2)is more hydrophobic than pure birnessite-MnO_(2),which is beneficial to prohibiting Mn dissolution and other side reactions.As a result,the elaborate design realizes effective transformation from low valence to high valence Mn for high capacity(291 mAh·g^(−1))and protective bambooslike structure for rate capacity(126 mAh·g^(−1)at 5 A·g^(−1))and cycling stability(89%capacity retention after 2,000 cycles).The assembled flexible quasi-solid-state Mn-Zn pouch batteries display application prospects for wearable and implantable electronic devices.The atomic engineering promoting Electrooxidation kinetics strategy will be instructive in activating other cathode materials and maximizing their capacity.

关键词： atomic engineering Mn-based cathode Electrooxidation Zn-ion battery long lifespan

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Late-stage azolation of benzylic C‒H bonds enabled by Electrooxidation

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Science China Chemistry 2021年第5期64卷 800-807页

作者： Zhixiong Ruan Zhixing Huang Zhongnan Xu Shaogao Zeng Pengju Feng Ping-Hua Sun Key Laboratory of Molecular Target&Clinical Pharmacology and the State Key Laboratory of Respiratory Disease School of Pharmaceutical Sciences&the Fifth Affiliated HospitalGuangzhou Medical UniversityGuangzhou 511436China International Cooperative Laboratory of Traditional Chinese Medicine Modernization and Innovative Drug Development of Chinese Ministry of Education College of PharmacyJinan UniversityGuangzhou 510632China Department of Chemistry Jinan UniversityGuangzhou 510632China

The installation of azoles via C–H/N–H cross-coupling is significantly underdeveloped,particularly in benzylic C–H azolation due to the requirement for external chemical oxidants and the challenge in controlling the site-and chemo-selectivity.Herein,a late-stage azolation of benzylic C‒H bonds enabled by Electrooxidation is described,which proceeds in an undivided cell under mild,catalyst-and chemical-oxidant-free reaction conditions.The strategy empowers the C‒H azolation on primary,secondary,and even challenging tertiary benzylic positions selectively.The remarkable synthetic utility of our approach is highlighted by its easy scalability without overoxidation of products and ample scope with valuable functional groups.The approach can be directly used to install benzyl and azole motifs on highly functionalized drug molecules.

关键词： Electrooxidation azolation external oxidant-free cross-dehydrogenative coupling late-stage functionalization

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Facile fabrication of PdRuPt nanowire networks with tunable compositions as efficient methanol Electrooxidation catalysts

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Nano Research 2018年第8期11卷 4348-4355页

作者： Changshuai Shang Yaxiao Guo Erkang Wang State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of SciencesChangchun 130022 China University of Chinese Academy of Sciences Beijing 100049 China

The preparation of nanomaterials with superior catalytic properties through simple and rapid protocols is a task of great importance. In the present study, we demonstrate the direct synthesis of trimetaUic PdRuPt nanowire networks through the reduction of the corresponding metal precursors with NaBH4, in the presence of KBr and polyvinylpyrrolidone （PV-P）. The elemental composition of the final products could be easily tuned by varying the added amounts of metal precursors. The obtained nanomaterials were then used as catalysts for methanol Electrooxidation in an acidic medium. Among the synthesized PdRuPt and PtPd nanowire networks, Pd0.97Ru0.44Pt exhibits the highest catalytic activity and durabili~ along with a specific activity 3.5 times higher than that of commercial Pt/C. The enhanced catalytic properties of the present nanowire systems are attributed to their unique structures and the introduction of Ru into PtPd nanocrystals with outstanding properties.The preparation of nanomaterials with superior catalytic properties through simple and rapid protocols is a task of great importance. In the present study, we demonstrate the direct synthesis of trimetaUic PdRuPt nanowire networks through the reduction of the corresponding metal precursors with NaBH4, in the presence of KBr and polyvinylpyrrolidone （PV-P）. The elemental composition of the final products could be easily tuned by varying the added amounts of metal precursors. The obtained nanomaterials were then used as catalysts for methanol Electrooxidation in an acidic medium. Among the synthesized PdRuPt and PtPd nanowire networks, Pd0.97Ru0.44Pt exhibits the highest catalytic activity and durability along with a specific activity 3.5 times higher than that of commercial Pt/C. The enhanced catalytic properties of the present nanowire systems are attributed to their unique structures and the introduction of Ru into PtPd nanocrystals with outstanding properties.

关键词： palladium ruthenium platinum nanowire networks methanol Electrooxidation

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Highly efficient and stable Electrooxidation of methanol and ethanol on 3D Pt catalyst by thermal decomposition of In2O3 nanoshells

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Journal of Energy Chemistry 2017年第1期26卷 193-199页

作者： Yuhang Xie Hulin Zhang Guang Yao Saeed Ahmed Khan Xiaojing Cui Min Gao Yuan Lin State Key Laboratory of Electronic Thin Film and Integrated Devices University of Electronic Science and Technology of ChinaChengdu 610054SichuanChina Center for Information in Medicine University of Electronic Science and Technology of ChinaChengdu 610054SichuanChina The First Sub-Institute Nuclear Power Institute of ChinaChengdu 610041SichuanChina

In this paper In2O3nanoshells have been synthesized via a facile hydrothermal approach. The nanoshells can be completely cracked into pony-size nanocubes by annealing, which are then used as a support of Pt catalyst for methanol and ethanol electrocatalytic oxidation. The prepared In2O3and supported Pt catalysts (Pt/In2O3) were characterized by X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), field effect scanning electron microscopy (FESEM), and transmission electron microscopy (TEM). Cyclic voltammetry (CV), linear sweep voltammetry (LSV), chronoamperometry and electrochemical impedance spectroscopy (EIS) were carried out, indicating the excellent catalytic performance for alcohol Electrooxidation can be achieved on Pt/In2O3nanocatalysts due to the multiple active sites, high conductivity and a mass of microchannels and micropores for reactant diffusions arising from 3D frame structures compared with that on the Pt/C catalysts. ? 2016 Science Press

关键词： Alcohols Catalyst activity Catalysts Chronoamperometry Cyclic voltammetry Decomposition Electrocatalysis Electrochemical impedance spectroscopy Electron microscopy Electrooxidation Energy dispersive spectroscopy Ethanol High resolution transmission electron microscopy Methanol Nanoshells Nanostructured materials Nanostructures Platinum Scanning electron microscopy Transmission electron microscopy X ray diffraction X ray photoelectron spectroscopy X ray spectroscopy

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Deciphering dynamic surface of PtRu alloy nanocatalysts to revisit their synergistic effects during the Electrooxidation

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Science China Chemistry 2024年第7期67卷 2224-2233页

作者： Xiao-Chong Li Bo Wang Zhou Yu Qiang Wan Ju-Fang Zheng Emmanuel Maisonhaute Xiao-Shun Zhou Ya-Hao Wang Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Institute of Physical ChemistryZhejiang Normal University Laboratoire Interface et Systèmes Electrochimiques CNRS UMR 8235Sorbonne Université

Correlating dynamic structural transformation of catalysts with the surface intermediate species under operating conditions is critical for updating the understanding of structure–performance relationships.Here,we probe the electrochemical potentialdependent surface structures and adsorbed intermediates on PtRu binary alloy nanocatalysts to revisit its synergistic mechanisms for CO Electrooxidation enhanced activity.In-situ spectral characteristics by using modified shell-isolated nanoparticle-enhanced Raman spectroscopy,show that in acidic solution,when the potential is positively scanned from 0.1 V to 1.5 V relative to reversible hydrogen electrode(RHE),the surface of the alloy catalyst evolves from metallic PtRu to adsorbed oxygen gradually covering and accumulating on Ru sites(denoted as PtRuOx,x≤2),forming segregated RuO2,and finally forming a threedimensional oxide layer(denoted as 3D PtRuO4).Moreover,molecular evidence associated with periodic density functional theory calculations reveals that electronic effects promote ruthenium to become more oxidizable and oxophilic.In particular,we found here that ~*O and ~*OH at surface RuOxsites are highly efficient CO oxidation active species in comparison to the same entities adsorbed on metallic Ru sites.This work sheds light on the complex surface dynamic process of practical Pt-based binary nanocatalysts and improves the understanding of synergistic mechanism for the development of fuel cell devices.

关键词： in-situ Raman spectroscopy surface evolution bifunctional mechanism PtRu Electrooxidation

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Facile growth of ultra-small Pd nanoparticles on zeolite-templated mesocellular graphene foam for enhanced alcohol Electrooxidation

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Nano Research 2019年第2期12卷 351-356页

作者： Xuexue Cui Yaling Li Mingyu Zhao Yunshi Xu Leilei Chen Shuguang Yang Yi Wang Center for Advanced Low-dimension Materials State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and Engineering Donghua University Shanghai 201620 China College of Chemistry Chemical Engineering and Biotechnology Donghua University Shanghai 201620 China

Labor-saving preparation of highly active electrocatalysts for alcohols oxidation, especially for the ethylene glycol and glycerol Electrooxidation is of great importance for the development of fuel cells. Herein, mesocellular graphene foam (MGF) constructed by ultrathin nanosheets were prepared using lamellar MCM-22 zeolite as template and then ultra-small Pd NPs were facile grew on it via the stabilizer-free synthesis. Detailed characterizations showed that the obtained Pd/MGF had large surface area, hierarchical porous architecture, semi-graphitic framework and dispersed Pd NPs an chori ng. Electrochemical measurements dem on strated that Pd/MGF possessed the higher catalytic activity (1.7-2.9 fold higher) and stability for the different alcohols Electrooxidation, especially for the ethylene glycol and glycerol Electrooxidation in the alkaline solution, than the commercial Pd/C (10 wt.%) catalyst. Reaction kinetics analysis revealed the expanded diffusion-controlled process of Pd/MGF as compared to Pd/C. These findings promised a potential electrocatalyst for direct alcohol fuel cells (DAFC), especially for the direct ethylene glycol or glycerol fuel cells with high energy density.

关键词： mesocellular graphene foam ultra-small nanoparticles stabilizer-free synthesis alcohol Electrooxidation reaction kinetics

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Effects of Lanthanide Ions on Electrooxidation of Methanol

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Chemical Research in Chinese Universities 2008年第5期24卷 632-634页

作者： WANG Hai-tao YIN Yu-chun GAO Shu-juan College of Chemical Engineering Northeast Dianli University Jilin 132012 P. R. China

Four kinds of lanthanide ions（Sm^3＋,Yb^3＋,Eu^3＋,La^3＋）as an additive were added into the aqueous solution containing methanol,respectively,and their effects on methanol elecotrooxidation in aqueous solutions were studied with cyclic voltammetry.The results show that the four kinds of ions have promotion action upon the Electrooxidation of methanol to different degrees.The best additive,Sm^3＋,can increase the anodic oxidation current of methanol by 80%and the peak potential shifted negatively about 50 mV.The promotion effects of the lanthanide ions were considered to be related to the extranuclear electron distribution of these ions and their adsorption on the Pt electrode surface.

关键词： Methanol Electrooxidation Lanthanide ion

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Electrooxidation of Hydroxypivalaldehyde in an Undivided Cell

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Chemical Research in Chinese Universities 2006年第5期22卷 626-630页

作者： YU Jian-guo CAO Xue-jing ZHANG Heng-bin ZHANG Yu-min LI Ke-chang College of Chemistry Jilin University Changchun 130021 P. R. China

The factors affecting the Electrooxidation of hydroxypivalaldehyde（HPAL） in an undivided cell were studied by using cyclic voltammetry（CV）, linear scan voltammetry（ LSV）, and potentiostatic electrolysis. The electrocatalytic activity and stability of a PbO2 electrode in sulfuric acid, acetic acid, and phosphoric acid were studied. The selectivity and the current efficiency for producing hydroxypivalic acid were explored with different supporting electrolytes, concentrations of HPAL, and pH values. The results show that higher selectivity and current efficiency for producing hydroxypivalic acid can be achieved when sulfuric acid with a high concentration is used as the supporting electrolyte and the selectivity and the current efficiency can reach 80% and 60%. resvectively.

关键词： Hydroxypivalaldehyde Hydroxypivalic acid Electrooxidation Electrosynthesis

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Effect Factors in Synthesis of Nicotinic Acid by Electrooxidation of 3-Picoline

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Chemical Research in Chinese Universities 2005年第6期21卷 692-696页

作者： SUN Xiu-yun ZHANG Yu-min CAO Xue-jing ZHANG Heng-bin LI Fei XU Yu-ling College of Chemistry Jilin University Changchun 130021 P. R. China Department of Applied Chemistry Jilin Institute of Chemical Technology Jilin 132022 P. R. China

In an electrolytic cell with a proton exchange membrane, nicotinic acid was synthesized at the PbO2 anode. The relationship between the current density and the potential at different concentrations of 3-picoline and sulfuric acid as well as at different temperatures was studied with polarization curves. The effects of the concentrations of sulfuric acid and 3-picoline, the anode potential and the reaction temperature on the selectivity and the current efficiency were explored. The optimum conditions were determined by orthogonal experiments. Under optimum conditions the selectivity and the current efficiency for the synthesis of nicotinic acid might reach 89% and 65%, respectively. The, concentrations of 3-picoline and nicotinic acid were analyzed with high performance liquid chromatography and the product was characterized with elemental analysis, chromatography-mass spectrometry and IR spectrometry.

关键词： 3-Picoline Nicotinic acid Electrooxidation Electroorganic synthesis

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