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Amino acids modified nanoscale zero-valent iron:Density functional theory calculations,experimental synthesis and application in the Fenton-like degradation of organic solvents

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Journal of Environmental Sciences 2024年第1期135卷 296-309页

作者： Xingchen Yang Fucheng Ming Jianlong Wang Lejin Xu Department of Nuclear Engineering and Technology School of Energy and Power EngineeringHuazhong University of Science and TechnologyWuhan 430074China China-EU Institute for Clean and Renewable Energy Huazhong University of Science and TechnologyWuhan 430074China Institute of Nuclear and New Energy Technology Key Laboratory of Advanced Reactor Engineering and Safety of Ministry of EducationTsinghua UniversityBeijing 100084China beijing key laboratory of radioactive wastes treatment Tsinghua UniversityBeijing 100084China

To improve the adsorption and catalytic performance of heterogeneous Fenton-like catalysts for oil wastes,amino acids were used to modify nanoscale zero-valent iron(AA@Fe^(0)),which were applied in the Fenton-like degradation of organic solvents(tributyl phosphate and n-dodecane,named TBP and DD).Twelve amino acids,i.e.,glycine(Gly),alanine(Ala),leucine(Leu),proline(Pro),phenylalanine(Phe),methionine(Met),cysteine(Cys),asparagine(Asn),serine(Ser),glutamic acid(Glu),lysine(Lys)and arginine(Arg),were selected and calculated by density functional theory(DFT).The optimized structure,charge distribution,the highest occupied molecular orbital(HOMO),the lowest unoccupied molecular orbital(LUMO),interaction region indicator(IRI)isosurface map and adsorption energy of AA@Fe^(0),AA@Fe^(0)-TBP and AA@Fe^(0)-DD were studied,which indicated that Fe is more likely to approach and charge transfer with-COO and-NH_(3) on theα-carbon of amino *** is strong attraction between Fe and–COO,and Van der Waals force between Fe and-NH_(3),*** the interaction of AA@Fe^(0)with TBP and DD,Van der Waal force plays an important ***@Fe^(0)was synthesized in laboratory and characterized to investigate physicochemical *** Fenton-like degradation of organic solvents,the change of COD in water phase during the degradation process as well as the volume of the organic phase after the reaction were *** results of calculations combined with experiments showed that Ser-modified Fe^(0)performed the best in these amino acids,with 98%removal of organic solvents.A possible catalytic mechanism was proposed in which amino acids acted a linking role between Fe and organic solvents,activating H_(2)O_(2)to generate hydroxyl radicals for the degradation of organic solvents.

关键词： Amino acids Nanoscale zero-valent iron Density functional theory Organic solvents Fenton-like degradation

Macroscopic polarization enhancement boosting piezo-photocatalytic performance via Nb-doping on B-site of Bi_(4)Ti_(3)O_(12)nanosheets

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Journal of Advanced Ceramics 2024年第4期13卷 437-446页

作者： Hongjian Yu Xindong Wei Min Wang Yan Zhang Zheng Wu Fan Guo Jie Han School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China Engineering Research Center of Ministry of Education for Geological Carbon Storage and Low Carbon Utilization of Resources Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid WastesNational Laboratory of Mineral MaterialsSchool of Material Sciences and TechnologyChina University of Geosciences(Beijing)Beijing 100083China School of Environmental and Chemical Engineering Xi’an Key Laboratory of Textile Chemical Engineering AuxiliariesXi'an Polytechnic UniversityXi'an 710048China

The development of a high-performance ferroelectric piezo-photocatalyst is an efficient strategy for advancing sustainability within the environmental and energy ***,a major challenge lies in the creation of a strong polarized electric field that can effectively hinder charge recombination,both within the bulk and on the surface of ***,we synthesize a series of Nb-doped Bi_(4)Ti_(3)O_(12)nanosheets via a facile one-pot hydrothermal method to achieve synergistically enhanced piezo-photocatalytic performance in CO_(2)reduction and pollutant *** optimized doped Bi_(4)Ti_(3)O_(12)demonstrates remarkable efficiency in the conversion of CO_(2)into CO,with a high production rate of 72.7μmol∙g−1∙h−1 without using co-catalysts or any sacrificial agent,surpassing the performance of unmodified Bi_(4)Ti_(3)O_(12)by up to 4.69 ***,our catalyst demonstrates ultra-fast piezo-photocatalytic degradation of organic pollutant Rhodamine B(RhB)at low concentrations and exceptional piezo-photocatalytic activity at high concentrations,outperforming most previously reported state-of-the-art *** systematic corroboration of catalyst characterization and experimental analysis reveals that the synergistic effect arises from the amplified macroscopic polarization induced by lattice distortion caused by the larger Nb ions,thereby improving piezo-photocatalytic *** research thus offers valuable insights into the direct design and fabrication of versatile catalytic systems,with applications spanning CO_(2)valorization and beyond.

关键词： CO_(2)reduction dye degradation piezo-photocatalysis Nb-doped Bi_(4)Ti_(3)O_(12) macroscopic polarization regulation

Insights into the mechanism of multiple Cu-doped Co Fe_(2)O_(4)nanocatalyst activated peroxymonosulfate for efficient degradation of Rhodamine B

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Journal of Environmental Sciences 2024年第3期137卷 382-394页

作者： Yuanmin Mo Xiaoping Zhang School of Environment&Energy South China University of TechnologyGuangzhou Higher Education Mega CentreGuangzhou 510006China The key laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters of Ministry of Education Guangzhou 510006China Guangdong Provincial key laboratory of Solid wastes Pollution Control and Recycling Guangzhou 510006China Guangdong Provincial Engineering and Technology Research Center for Environmental Risk Prevention and Emergency Disposal Guangzhou 510006China

The multiple metal catalyst as a promising nanomaterial has shown excellent activity in the peroxymonosulfate(PMS)activation for pollutant ***,the role of special sites and in-depth understanding of the PMS activation mechanism are not fully *** this study,a Cu-doped CoFe_(2)O_(4)nanocatalyst(0.5CCF)was synthesized by a sol-gel and calcination method,and used for PMS activation to remove Rhodamine B(RhB).The results showed that the Cu doping obviously enhanced the catalytic performance of CoFe_(2)O_(4),with 99.70%of RhB removed by 0.5CCF while 74.91%in the CoFe_(2)O_(4)within 15 *** on the X-ray photoelectron spectroscopy and electrochemical analysis,this could be ascribed to the more low valence of Co and Fe species generated on the 0.5CCF and faster electron transfers occurred in the 0.5CCF due to the Cu *** addition,Cu doping could provide more reaction sites for the 0.5CCF to activate PMS for RhB *** metal species and the surface hydroxyl were the reaction sites of PMS activation,and the surface hydroxyl played an important role in surface-bound reactive species *** the PMS activation,the Cu not only activated PMS to produce reactive oxygen species(ROS),but also regenerated Co^(2+)and Fe^(2+)to accelerate the PMS *** non-radical of ^(1)O_(2)was the main ROS with a 99.35%of contribution rate,and the SO_(5)^(·–)self-reaction was its major *** study provides a new insight to enhance the PMS activation performance of multiple metal catalysts by Cu doping in wastewater treatment.

关键词： Cu-doped CoFe_(2)O_(4)nanocatalyst PMS activation Mechanism Rhodamine B removal

Study on synergistic leaching of potassium and phosphorus from potassium feldspar and solid waste phosphogypsum via coupling reactions

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Chinese Journal of Chemical Engineering 2024年第1期65卷 117-129页

作者： Chao Li Shizhao Wang Yunshan Wang Xuebin An Gang Yang Yong Sun School of Chemical Engineering and Technology Hebei University of TechnologyTianjin 300130China National Engineering Research Center of Green Recycling for Strategic Metal Resources Chinese Academy of SciencesBeijing 100190China School of Engineering Edith Cowan University270 Joondalup DriveJoondalupWA 6027Australia key laboratory of Carbonaceous wastes Processing and Process Intensification of Zhejiang Province The University of Nottingham Ningbo ChinaNingbo 315100China

To achieve the resource utilization of solid waste phosphogypsum(PG)and tackle the problem of utilizing potassium feldspar(PF),a coupled synergistic process between PG and PF is proposed in this *** study investigates the features of P and F in PG,and explores the decomposition of PF using hydrofluoric acid(HF)in the sulfuric acid system for K leaching and leaching of P and F in *** impact factors such as sulfuric acid concentration,reaction temperature,reaction time,material ratio(PG/PF),liquid–solid ratio,PF particle size,and PF calcination temperature on the leaching of P and K is systematically investigated in this *** results show that under optimal conditions,the leaching rate of K and P reach more than 93%and 96%,*** study using shrinking core model(SCM)indicates two significant stages with internal diffusion predominantly controlling the leaching of *** apparent activation energies of these two stages are 11.92 kJ·mol^(-1)and 11.55 kJ·mol^(-1),respectively.

关键词： Phosphogypsum Potassium feldspar Coupling reaction Leaching Waste treatment Kinetics

Singlet oxygen-dominated peroxymonosulfate activation by layered crednerite for organic pollutants degradation in high salinity wastewater

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Journal of Environmental Sciences 2024年第1期135卷 86-96页

作者： Chengji Sui Zixuan Nie Huan Liu Grzegorz Boczkaj Weizhen Liu Lingshuai Kong Jinhua Zhan key laboratory for Colloid&Interface Chemistry of Education Ministry Department of ChemistryShandong UniversityJinan 250100China School of Environment and Energy Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and RecyclingSouth China University of TechnologyGuangzhou 510006China Gdansk University of Technology Faculty of Civil and Environmental EngineeringDepartment of Sanitary EngineeringG.Narutowicza St.11/1280-233 GdanskPoland EkoTech Center Gdansk University of TechnologyG.Narutowicza St.11/1280-233 GdanskPoland

Advanced oxidation processes have been widely studied for organic pollutants treatment in water,but the degradation performance of radical-dominated pathway was severely inhibited by the side reactions between the anions and radicals,especially in high salinity ***,a singlet oxygen(^(1)O_(2))-dominated non-radical process was developed for organic pollutants degradation in high salinity wastewater,with layered crednerite(CuMnO_(2))as catalysts and peroxymonosulfate(PMS)as *** on the experiments and density functional theory calculations,^(1)O_(2)was the dominating reactive species and the constructed Cu-O-Mn with electron-deficient Mn captured electron from PMS promoting the generation of^(1)O_(2).The rapid degradation of bisphenol A(BPA)was achieved by CuMnO_(2)/PMS system,which was 5-fold and 21-fold higher than that in Mn_(2)O_(3)/PMS system and Cu_(2)O/PMS *** CuMnO_(2)/PMS system shown prominent BPA removal performance under high salinity conditions,prominent PMS utilization efficiency,outstanding total organic carbon removal rate,wide range of applicable pH and good *** work unveiled that the^(1)O_(2)-dominated non-radical process of CuMnO_(2)/PMS system overcame the inhibitory effect of anions in high salinity conditions,which provided a promising technique to remove organic pollutants from high saline wastewater.

关键词： Singlet oxygen Non-radical process High salinity Mixed metal oxides Wastewater treatment

Risk stratification for radioactive iodine refractoriness using molecular alterations in distant metastatic differentiated thyroid cancer

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Chinese Journal of Cancer Research 2024年第1期36卷 25-35页

作者： Zhuanzhuan Mu Xin Zhang Dongquan Liang Jugao Fang Ge Chen Wenting Guo Di Sun Yuqing Sun Zhentian Kai Lisha Huang Jun Liang Yansong Lin Department of Nuclear Medicine State Key Laboratory of Complex Severe and Rare DiseasesPeking Union Medical College(PUMC)HospitalChinese Academy of Medical Sciences&PUMCBeijing 100730China beijing key laboratory of Molecular Targeted Diagnosis and Therapy in Nuclear Medicine Beijing 100730China Pepperdine University Graduate School of Education and Psychology Los Angeles 90045USA Department of Head and Neck Surgery Affiliated Beijing Tongren HospitalCapital Medical UniversityBeijing 100730China Department of General Surgery State Key Laboratory of Complex Severe and Rare DiseasesPeking Union Medical College(PUMC)HospitalChinese Academy of Medical Sciences&PUMCBeijing 100730China Central laboratory State Key Laboratory of Complex Severe and Rare DiseasesPeking Union Medical College(PUMC)HospitalChinese Academy of Medical Sciences&PUMCBeijing 100730China Department of Bioinformatics Zhejiang Shaoxing Topgen Biomedical Technology Co.LtdShanghai 201321China Department of Medicine Zhejiang Shaoxing Topgen Biomedical Technology Co.LtdShanghai 201321China Department of Oncology Peking University International HospitalBeijing 102206China

Objective: Patients with radioactive iodine-refractory differentiated thyroid cancer(RAIR-DTC) are often diagnosed with delay and constrained to limited treatment options. The correlation between RAI refractoriness and the underlying genetic characteristics has not been extensively ***: Adult patients with distant metastatic DTC were enrolled and assigned to undergo next-generation sequencing of a customized 26-gene panel(Thyro Lead). Patients were classified into RAIR-DTC or non-RAIR groups to determine the differences in clinicopathological and molecular characteristics. Molecular risk stratification(MRS) was constructed based on the association between molecular alterations identified and RAI refractoriness, and the results were classified as high, intermediate or low ***: A total of 220 patients with distant metastases were included, 63.2% of whom were identified as RAIRDTC. Genetic alterations were identified in 90% of all the patients, with BRAF(59.7% vs. 17.3%), TERT promoter(43.9% vs. 7.4%), and TP53 mutations(11.5% vs. 3.7%) being more prevalent in the RAIR-DTC group than in the non-RAIR group, except for RET fusions(15.8% vs. 39.5%), which had the opposite pattern. BRAF and TERT promoter are independent predictors of RAIR-DTC, accounting for 67.6% of patients with RAIR-DTC. MRS was strongly associated with RAI refractoriness(P<0.001), with an odds ratio(OR) of high to low MRS of 7.52 [95%confidence interval(95% CI), 3.96-14.28;P<0.001] and an OR of intermediate to low MRS of 3.20(95% CI,1.01-10.14;P=0.041).Conclusions: Molecular alterations were associated with RAI refractoriness, with BRAF and TERT promoter mutations being the predominant contributors, followed by TP53 and DICER1 mutations. MRS might serve as a valuable tool for both prognosticating clinical outcomes and directing precision-based therapeutic interventions.

关键词： Differentiated thyroid cancer distant metastases genetic alterations RAI refractoriness molecular risk stratification

New insight into polystyrene ion exchange resin for efficient cesium sequestration:The synergistic role of confined zirconium phosphate nanocrystalline

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Chinese Chemical Letters 2024年第1期35卷 406-411页

作者： Mengzhou Wang Mingyan Fu Junfeng Li Yihui Niu Qingrui Zhang Qina Sun Hebei key laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse School of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004China laboratory of Environmental Technology INETTsinghua UniversityBeijing 100084China

Polystyrene resins(PS)have been practical ion exchangers for radionuclides removal from ***,nonspecific effects of ion exchange groups continue to be a major obstacle for emergency treatment with coexisting ions of high *** selectivity for Cs+enables zirconium phosphate(ZrP)to be the most promising inorganic sorbent for radioactive cesium extraction,despite being difficult to synthesize and causing excessive pressure loss in fixed-bed reactors due to fine ***,through facile confined crystallization in host macropores,we prepared PS confinedα-ZrP nanocrystalline(ZrP-PS).Size-screen sorption of layeredα-ZrP and sulfonic acid group preconcentration of PS synergistically enable a considerably higher Cs+affinity of ZrP-PS than PS,as confirmed by X-ray photoelectron spectroscopy(XPS)***-PS demonstrated remarkable cesium sequestration performance in both batch and continuous experiments,with a high adsorption capacity of 269.58 mg/g,a rapid equilibrium within 80 min,and a continuous effluent volume of 2300 L/kg *** the excellent selectivity for Cs+and flexibility to separate from treated water,ZrP-PS holds great promise as purification packages for the emergency treatment of radioactively contaminated water.

关键词： Zirconium phosphate Nanocrystalline Polystyrene resin Cesium Removal

Black phosphorus-based heterostructures for photocatalysis and photoelectrochemical water splitting

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Journal of Energy Chemistry 2022年第4期31卷 745-779页

作者： Shutao Li Yihe Zhang Hongwei Huang beijing key laboratory of Materials Utilization of Nonmetallic Minerals and Solid wastes and School of Materials Science and Technology China University of GeosciencesBeijing 100083China

Semiconductor-based photocatalytic and photoelectrochemical(PEC) processes can convert solar energy into high-density chemical energy or for the treatment of environmental pollutants, which are ideal ways to deal with environmental and energy crises. The development of high-efficiency photocatalysts and photoelectrodes is the key to the in-depth development and practical application of the two *** phosphorus(BP) has excellent physicalcochemical properties such as adjustable band gap, high carrier mobility, large specific surface area and anisotropy, making it one of the most promising ***-based heterostructure can not only realize the effective separation of photogenerated carriers but also improve the stability of BP, and is widely used in photocatalytic and PEC reactions. In this review, we first introduce the crystal structure, band structure, anisotropy, and preparation of BP with different dimensions(bulk, zero-dimension and two-dimension). Then, according to the transfer path of the photogenerated carriers and the components, the BP-based heterostructures are divided into type I heterojunction, type II heterojunction, Z-scheme heterojunction, S-scheme heterojunction, BP/carbonbased material heterostructure, BP/metal heterostructure and multi-component *** are the diverse photocatalytic applications of BP-based heterostructure, such as water splitting and CO_(2)reduction, N_(2)fixation, pollutant degradation, photothermal and photodynamic ***, some concluding views and opinions are stated on the challenges and opportunities faced by the further development of BP-based heterostructures in photocatalysis and PEC water splitting.

关键词： Black phosphorus Heterostructure Photocatalysis Photoelectrochemical water splitting

MOF-derived spherical Ni_(x)S_(y)/carbon with B-doping enabling high supercapacitive performance

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Journal of Materials Science & Technology 2023年第22期153卷 219-227页

作者： Jingjing Hu Yan Shi Li Sun Feng Xie Kaiyue Gao Yaru Qu Hankun Tan Yihe Zhang beijing key laboratory of Materials Utilization of Nonmetallic Minerals and Solid wastes National Laboratory of Mineral MaterialsSchool of Materials Science and TechnologyChina University of GeosciencesBeijing 100083China

This work uses a simple Ni-metal organic framework(Ni-MOF)to generate a uniform metal-containing carbon hybrid structure of Ni/C by in-situ ***,after NaBH_(4) treatment and hydrothermal vul-canization of Ni/C,multiphase B-doped Ni_(x)S_(y) nanoparticles can be obtained and uniformly anchored in the carbon skeleton,forming a highly porous flower-shaped B-Ni_(x)S_(y)/C *** positive role of B doping was theoretically confirmed by Density Function Theory(DFT)*** MOF-derived car-bon framework has porous,conductive,and continuous features beneficial for fast charge *** are also multiple Ni-sulfide phases in B-Ni_(x)S_(y)/C,dominated by hexagonal NiS,hexagonal Ni 2 S 3,and cu-bic Ni_(3)S_(4),which give rich valance state and are expected to bring active electrochemical *** addition,the boronation process by the reducing agent of NaBH_(4) is also proved beneficial to bring high capacitance,possibly due to the incorporation of more active sites by ***,the B-Ni_(x)S_(y)/C compos-ite electrode delivers a high specific capacity of 1250.4 C g^(-1) at 1 A g^(-1) and excellent rate *** B-Ni_(x)S_(y)/C-based asymmetric supercapacitor also shows promising prospects for future energy stor-age devices,delivering high cyclability with capacitance retention of 87.6%after 7000 *** work proves the efficiency of MOF-derived carbon framework and B-doping in improving metal sulfide’s electrochemical performances.

关键词： B-Ni_(x)S_(y)/C Carbon skeleton Flower-shaped Hybrid capacitor Asymmetric supercapacitor