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A Binary Dumbbell Visible Light Driven Photocatalyst for Simultaneous Hydrogen Production with the Selective Oxidation of Benzyl Alcohol to Benzaldehyde

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SSRN 2024年

作者： Tayyab, Muhammad Mansoor, Seemal Akmal, Zeeshan Khan, Mazhar Zhou, Liang Lei, Juying Zhang, Jinlong Key Laboratory for Advanced Materials Shanghai Engineering Research Center for Multimedia Environmental Catalysis and Resource Utilization Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research Center School of Chemistry and Molecular Engineering East China University of Science and Technology Shanghai200237 China Institute of Materials Research Tsinghua Shenzhen International Graduate School Tsinghua University Guangdong Shenzhen518055 China National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process East China University of Science and Technology Shanghai200237 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China State Key Laboratory of Urban Water Resource and Environment Harbin Institute of Technology Harbin150090 China

Photocatalytic H2 production with selective oxidation of organic moieties in an aqueous medium is a fascinating research area. However, the rational design of photocatalysts and their photocatalytic performance are still inadequate. In this work, we efficiently synthesized the MoS2 tipped CdS nanowires (NWs) photocatalyst using soft templates via the two-step hydrothermal method for efficient H2 production with selective oxidation of benzyl alcohol (BO) under visible light illumination. The optimized MoS2 tipped CdS NWs (20% MoS2) photocatalyst exhibits the highest photocatalytic H2 production efficiency of 13.55 mmol g-1 h-1 with 99% selective oxidation of BO, which was 42.34 and 2.21 times greater photocatalytic performance than that of pristine CdS NWs and MoS2/CdS NWs, respectively. The directional loading of MoS2 at the tips of CdS NWs (as compared to nondirectional MoS2 at CdS NWs) is the key factor towards superior H2 production with 99% selective oxidation of BO and has an inhibitory effect on the photo corrosion of pristine CdS NWs. Therefore, the amazing enhancement in the photocatalytic performance and selectivity of optimized MoS2 tipped CdS NWs (20% MoS2) photocatalyst is due to the spatial separation of their photoexcited charge carriers through the Schottky junction. Moreover, the unique structure of MoS2 flower at the tip of 1D CdS NWs offers separate active sites for adsorption and surface reactions such as H2 production at the MoS2 flower (confirmed by Pt photo deposition) and subsequently the selective oxidation of BO at the stem of CdS NWs. This rational design of a photocatalyst could be an inspiring work for the further development of efficient photocatalytic system for H2 production with selective oxidation of BO (a strategy of mash two potatoes with one fork). © 2024, The Authors. All rights reserved.

关键词： Precious metals

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Cyanometallate Framework Templated Synthesis of Hierarchically Porous La(Oh)3 for High-Efficient and Stable Phosphorus Removal from Tailwater

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SSRN 2023年

作者： Jing, Xiaoxu Zhang, Jing Li, Yungui Li, Qingqing Shen, Yi Zhang, Suorong Fang, Qile Advanced Institute of Natural Sciences Beijing Normal University Zhuhai519087 China Sichuan Provincial Sci-Tech Cooperation Base of Low-cost Wastewater Treatment Technology Department of Environmental Engineering Southwest University of Science and Technology Mianyang621010 China Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province College of Environment Zhejiang University of Technology Hangzhou310032 China Chongqing Feiyang Measurement and Control Technology Research Institute Co. Ltd Chongqing402760 China

Lanthanum (La)-based hydroxides have been recognized as promising candidates for dephosphorization due to their high affinity and selectivity for phosphate adsorption. However, the development of porous La(OH)3 materials with enriching active sites and high structural stability remains a challenge in tailwater treatment. Here we developed a novel self-templating method based on an ion-exchange mechanism to construct hierarchically porous La(OH)3, where the OH− of an alkali conversion reagent replaces the [Fe(CN)6]4− cluster within the LaFe cyanometalate (CM) precursor, simultaneously completing the hydroxide conversion and pore-creating processes. The obtained hierarchically porous La(OH)3 shows excellent structural stability with no ion leaching and can maintain its primary microsphere structure and secondary nanoneedle morphology after multiple cycles of application. Due to the abundant micropores/mesopores, there are fully exposed active sites inside and outside the porous La(OH)3 microsphere, giving it an excellent phosphate adsorption capacity (maximum capacity of 163.6 mg P/g). Its high selectivity and environmental adaptability make it a favorable adsorbent for aquaculture tailwater treatment that can rapidly reduce the dissolved inorganic phosphorus level to below 0.05 mg P/L to meet the mariculture tailwater discharge standard in a wide range of salinities and temperatures. The information gleaned in this study provides valuable guidance for the materials design of porous La-based hydroxides for phosphorus removal. © 2023, The Authors. All rights reserved.

关键词： Aquaculture

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Hierarchical Anion Exchange and Reverse Electron Transfer in Ldh/Peroxymonosulfate System for Roxarsone Elimination

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SSRN 2024年

作者： Pei, Wenkai Zheng, Yifan Gao, Jianyu Lei, Juying Liu, Yongdi Zhou, Liang Zhang, Jinlong Wang, Yu National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process East China University of Science and Technology Shanghai200237 China Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization Key Laboratory for Advanced Materials Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research Center School of Chemistry and Molecular Engineering East China University of Science and Technology 130 Meilong Road Shanghai200237 China Department of Molecular Engineering Graduate School of Engineering Kyoto University Kyoto-Daigaku Katsura Nishikyo-ku Kyoto615-8510 Japan State Key Laboratory of Urban Water Resource and Environment Harbin Institute of Technology Harbin150090 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China

Roxarsone (ROX) is the main form of As pollution in the world, and developing effective methods for its elimination is beneficial to human health and ecological environment. Herein, we report glutaraldehyde-crosslinked chitosan encapsulated CoCe-LDH as an outstanding catalyst for the advanced oxidation of ROX and the efficient adsorption of inorganic arsenic. 100% of ROX and more than 98.5% of As(III)/As(V) were eliminated, and over 99.3% of remained inorganic arsenic was oxidized to low toxicity As(V) in the PMS-activation system, and some specific properties of LDH are considered the main reasons. The hierarchical anion exchange has been confirmed to be beneficial for constructing a high concentration PMS inter layer microenvironment. And the unique reverse electron transfer process induced the 100% selective production of singlet oxygen. This work not only develops an advanced ROX removal method, but also provides a new understanding of LDH-based advanced oxidation process. © 2024, The Authors. All rights reserved.

关键词： Chemical activation

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Molecular Transformations of Dom, Don and Dos in Human-Impacted Estuarine Sediments

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SSRN 2023年

作者： Ni, Zhaokui Wu, Yue Ma, Yu Li, Yu Li, Dan Wang, Shengrui Zhou, Chunyang Guangdong-Hong Kong Joint Laboratory for Water Security Center for Water Research Advanced Institute of Natural Sciences Beijing Normal University Zhuhai519087 China Yunnan Key Laboratory of Pollution Process and Management of Plateau Lake-Watershed Kunming650034 China National Engineering Laboratory for Lake Pollution Control and Ecological Restoration Chinese Research Academy of Environmental Sciences Beijing100012 China College of Water Sciences Beijing Normal University Beijing100875 China College of Urban Construction Nanjing Tech University Nanjing211816 China

Estuaries are key active zones for global biogeochemical cycle of dissolved organic matter (DOM). However, understanding the DOM molecular transformation and spatial distribution pattern in estuarine sediments is challenging owning to complex biogeochemical processes and limitation of techniques. Herein, UV–visible, EEM fluorescence spectroscopy, FT-ICR MS and microbial high-throughput sequencing techniques were integrated to elucidate the molecular transformations and controlling mechanisms of DOM and nitrogen/sulfur-bearing DOM (DON, DOS) in sediments of the Pearl River Estuary (PRE). The results showed that the molecular chemo-diversities, properties, compositions and reactivities of sediment DOM, DON and DOS all displayed noticeable gradients along the river-estuary continuum. Sediment DOM in upper estuary is characterized by higher aromaticity, hydrophobicity and substitution group quantities. The molecular chemo-diversities of DOM, DON and DOS decreased from upper to lower estuary, whereas the molecular weights (MW) and instability (MLBL) increased. In addition, the relative abundance of tannin/lignin-like substances in DON/DOS decreased while the protein/lipid-like components increased. These indicate the increasing reactivity of sediment DOM, DON and DOS along river-estuary continuum. Multi-factor analysis suggested that the spatial transformations of DOM, DON and DOS in molecular properties, compositions and reactivities, were jointly shaped by sources, degradability and microbial activities. Besides, the anthropogenically derived N and S heteroatoms can enhance the MW and instability of DOM and may further accelerate DOM migration and transformation in estuarine sediments. This study provides molecular insights into the distinctive distribution patterns of DOM, DON and DOS in properties, compositions, and reactivities in estuarine sediments and will benefit the evaluation and predication framework concerning the impact of DOM cycles on environmental issues

关键词： Estuaries

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Multiple α sub-variants and anisotropic mechanical properties of an additively-manufactured Ti-6Al-4V alloy

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Journal of Materials Science & technology 2021年第11期70卷 113-124页

作者： Yinling Zhang Zhuo Chen Shoujiang Qu Aihan Feng Guangbao Mi Jun Shen Xu Huang Daolun Chen School of Materials Science and Engineering Tongji UniversityShanghai 201804China Department of Mechanical and Industrial Engineering Ryerson UniversityTorontoOntario M5B 2K3Canada Aerospace Hiwing(Harbin)Titanium Industrial Co. Ltd.Harbin High Tech ZoneHarbin 150028China Shanghai Key Lab.of D&A for Metal-Functional Materials School of Materials Science&EngineeringTongji UniversityShanghai 201804China Aviation Key Laboratory of Science and Technology on Advanced Titanium Alloys AECC Beijing Institute of Aeronautical MaterialsBeijing 100095China College of Mechatronics and Control Engineering Shenzhen UniversityShenzhen 518060China

Additive manu facturing(AM)is a promising material processing method which gains significant momentum in the aerospace and biomedical ***,the anisotropy in the mechanical properties of additively-manufactured materials is still poorly *** study was aimed at elucidating crystallographic feature-anisotropy-mechanical property relationship for a Ti-6Al-4V alloy manufactured via selective electron beam melting(SEBM).Abundantαlamellae with six variants were present inside the columnar prior-βgrains with a<100>fiber texture duringβ→αphase *** sixαvariants followed the Burgers orientation relationship of{110}_(β)//{0001}_(α)and<1-11>_(β)//<11-20>_(α).Multiple sub-variants in eachαvariant were observed for the first *** anisotropy in the mechanical properties was mainly related to the relative amount of sixα*** the horizontally-oriented samples had a lower yield strength,they exhibited a higher ductility and longer fatigue life than the vertically-oriented *** softening occurred at higher strain amplitudes,and cyclic stabilization sustained at lower strain *** crack mainly initiated from the specimen surface at lower strain amplitudes,while multiple crack initiation tended to occur at higher strain *** propagation was characterized by fatigue striations along with some secondary cracks.

关键词： Titanium alloy 3D printing Deformation behavior Anisotropy Burgers orientation relationship

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Simultaneous hydrogen production with the selective oxidation of benzyl alcohol to benzaldehyde by a noble‐metal‐free photocatalyst VC/CdS nanowires

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Chinese Journal of Catalysis 2022年第4期43卷 1165-1175页

作者： Muhammad Tayyab Yujie Liu Shixiong Min Rana Muhammad Irfan Qiaohong Zhu Liang Zhou Juying Lei Jinlong Zhang Key Laboratory for Advanced Materials Shanghai Engineering Research Center for Multi‐media Environmental Catalysis and Resource UtilizationJoint International Research Laboratory of Precision Chemistry and Molecular EngineeringFeringa Nobel Prize Scientist Joint Research CenterSchool of Chemistry and Molecular EngineeringEast China University of Science&TechnologyShanghai 200237China National Engineering Laboratory for Industrial Wastewater Treatment East China University of Science and TechnologyShanghai 200237China State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process East China University of Science and TechnologyShanghai 200237China School of Chemistry and Chemical Engineering North Minzu UniversityYinchuan 750021NingxiaChina College of Energy Soochow Institute for Energy and Materials Innovations(SIEMIS)Soochow UniversitySuzhou 215006JiangsuChina

In this work we used CdS NWs(nanowires)with vanadium carbide(VC)attached via facile electrostatic self‐assembly and calcination *** results showed that compared to pristine CdS NWs,the photocatalytic activity of CdS NWs loaded with the particular amount of VC was dramatically *** them,the VC/CS‐15 indicated the highest enhancement for simultaneous production of H2 with selective oxidation of benzyl alcohol(BO)into benzaldehyde(BD).The highest hydrogen evolution rate of 20.5 mmol g^(-1)h^(-1)was obtained with more than 99%selectivity for BD production under visible light(λ˃420 nm)irradiation for 2 h,which was almost 661 times higher than the pristine CdS *** enhancement of photocatalytic activity is due to the VC,which provides a favorable attraction for BO by lowering the zeta potential,along with the active site for hydrogen production,and retard the recombination of electron‐hole pairs by increasing the conductivity of the ***,the apparent quantum efficiency(AQE)of VC/CS‐15 for BD and H_(2)production at monochromatic 420 nm is about 7.5%.At the end of the hydrogen evolution test,the selective oxidation with more than 99%selectivity was *** hopes this work will prove its future significance and move scientific community toward a more economical way for achieving the commercialization of H_(2) by photocatalysis.

关键词： Hydrogen production Selective oxidation Benzaldehyde Noble‐metal‐free Visible light

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Comparative Study of Photocatalytic H2 Production by Nickel Chalcogenides1+x Based Zn3In2S6 Photocatalytic System

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SSRN 2024年

作者： Mansoor, Seemal Hu, Zixu Zheng, Yifan Tayyab, Muhammad Khan, Mazhar Akmal, Zeeshan Zhou, Liang Lei, Juying Zhang, Jinlong Key Laboratory for Advanced Materials Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research Center School of Chemistry and Molecular Engineering East China University of Science & Technology Shanghai200237 China National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process East China University of Science and Technology 130 Meilong Road Shanghai200237 China Department of Molecular Engineering Graduate School of Engineering Kyoto University Kyoto-Daigaku Katsura Nishikyo-ku Kyoto615-8510 Japan State Key Laboratory of Urban Water Resource and Environment Harbin Institute of Technology Harbin150090 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China Institute of Materials Research Tsinghua Shenzhen International Graduate School Tsinghua University Guangdong Shenzhen518055 China

Exploiting metal chalcogenide-based photocatalysts has fascinated researchers as a source of green hydrogen (H2) energy. Herein, we have designed a novel selenium-enriched NiSe1+x/ZIS (NiSexZ) photocatalytic system via a two-step hydrothermal and facile photo-deposition method. It was fascinating to conclude here that the NiSexZ photocatalytic system showed boosted H2 evolution results in comparison with other sulphur-enriched NiS1+x/ZIS (NiSxZ) and tellurium-enriched NiTe1+x/ZIS (NiTexZ). The optimized NiSe0.5Z composite exhibited a photocatalytic H2 evolution of 3.24 mmol g -1 h -1, a 9.8-fold increase over pure ZIS and it demonstrated an apparent quantum efficiency (AQE) of 2.06% via 420nm filter. Moreover, sulphur (S), selenium (Se), and tellurium (Te) synergistic active sites were exposed to promote H2 evolution reaction in this work. Given the significant advancements and commendable performance exhibited by the Se-Hads across the week bond, it is extremely probable that the NiSe1+x cocatalyst holds immense potential for the development of sophisticated photocatalytic materials. © 2024, The Authors. All rights reserved.

关键词： Nickel compounds

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Recursive Weighted Null-Space Fitting Method for Identification of Multivariate Systems ⁎

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IFAC-PapersOnLine 2021年第7期54卷 345-350页

作者： Mengyuan Fang Miguel Galrinho Håkan Hjalmarsson Zhejiang Engineering Laboratory of Industrial Internet Communication Technology Zhejiang Sci-Tech University Hangzhou China. State Key Laboratory of Synthetical Automation for Process Industries Northeastern University Shenyang China OHB Sweden AB Kista Sweden Centre for Advanced Bio Production and Division of Decision and Control Systems School of Electrical Engineering and Computer Science KTH Royal Institute of Technology Sweden

Recursive identification of structured multivariate models is known to be difficult due to the general non-convexity of the likelihood function. In this work, we propose a recursive multivariate weighted null-space fitting method for identification of structured multivariate models. The proposed method first uses recursive least squares to estimate a high order non-parametric model, then a parametric model is obtained through weighted least squares from the non-parametric model. In this way, the method avoids directly optimizing a non-convex likelihood function and has guaranteed global convergency. Moreover, the proposed method is flexible in model structures and has the same finite sample performance as its off-line counterpart. We use simulation examples to illustrate the performance.

关键词： Recursive system identification multivariate systems weighted null-space fitting

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Hexagon Flower-Shaped Architectures Constructed of Lanthanum Hydroxide Nanosheets for Superior Phosphate Removal: Synthesis and Mechanism Study

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SSRN 2023年

作者： Zhang, Jing Shen, Yi Liang, Chenge Yi, Huiyu Li, Qingqing Dong, Pingping Fang, Qile Li, Yungui Advanced Institute of Natural Sciences Beijing Normal University Zhuhai519087 China School of Environment Beijing Normal University Beijing100875 China Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province College of Environment Zhejiang University of Technology Hangzhou310032 China Sichuan Provincial Sci-Tech Cooperation Base of Low-cost Wastewater Treatment Technology Department of Environmental Engineering Southwest University of Science and Technology Mianyang621010 China Southwest University of Science and Technology China

In response to phosphorus pollution, developing functional materials for phosphate adsorption is an ideal method to reach an ultralow phosphate concentration in effluent. Herein, a hexagon flower-shaped architecture constructed of lanthanum (La)-based hydroxide nanosheets was fabricated from LaFe cyano-bridged metal frameworks (CMs) via a self-templating strategy using NH4‧H2O as the conversion reagent. The ion exchange process using weak alkaline reagent enables the formation of secondary nanosheets on the architecture, thus leading to a high surface area and a large number of mesopores that provide abundant active sites and mass transfer channels for phosphate adsorption. A superior adsorption capacity of 127.5 mg P/g can be obtained on the La-based architecture, which also shows satisfactory applicability over a wide pH range. A ligand exchange between -OH and phosphate ions is verified as the main adsorption mechanism, which properly accounts for its excellent selectivity for phosphate adsorption when coexisting with other anions/cations and natural organic matters. Overall, the present study provides a new method for constructing porous La-based hydroxide materials for phosphorus control in water. © 2023, The Authors. All rights reserved.

关键词： Nanosheets

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Activation of Peroxymonosulfate By Laco3oh Coupled with N, S Co-Doped Graphene for Levofloxacin Degradation

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SSRN 2023年

作者： Pei, Wenkai Wang, Yu Liu, Yujie Zhou, Liang Lei, Juying Zhang, Jinlong National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery School of Resources and Environmental Engineering East China University of Science and Technology Shanghai200237 China ShanghaiEngineeringResearchCenterforMulti-mediaEnvironmentalCatalysisandResourceUtilization East China University of Science and Technology 130 Meilong Road Shanghai200237 China Key Laboratory for Advanced Materials Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research Center School of ChemistryandMolecularEngineering EastChinaUniversityofScienceandTechnology 130MeilongRoad Shanghai200237 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China State Key Laboratory of Urban Water Resource and Environment Harbin Institute of Technology Harbin150090 China

The activation of peroxymonosulfate (PMS) by metal-based materials is currently considered to have great potential for pollutant treatment. However, secondary environmental damage from common transition metals is often unavoidable. Rare earth metals with high energy level, multi-electron configuration and unique 4f orbital can be used as an electron transfer bridge to reduce interfacial energy loss and promote electron transfer, which were incorporated the catalyst to activate PMS. In this study, calcination and hydrothermal method were combined to fabricated LaCO3OH coupled with N, S co-doped graphene(LCOH/GNS), which exhibited superior catalytic performance in PMS activation for LVX degradation. LaCO3OH(LCOH) was first used for PMS activation and showed excellent degradation properties and reduced ecotoxicity. The doping of N and S in the graphene matrix enhances the adsorption of PMS, electron transfer and reduces metal ion leaching, thus promoting the interaction and reaction between LCOH and PMS. The degradation process may involve multiple-oxidative pathways, which was confirmed by radical quenching experiments and the EPR technique. This study provided a novel method for the rational design of rare earth metal based-carbon catalysts, and LCOH/GNS-PMS was expected to be a promising technology for antibiotic degradation in wastewater treatment. © 2023, The Authors. All rights reserved.

关键词： Graphene

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