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Mechanism investigation of A-site doping on modulating electronic band structure and photocatalytic performance towards CO_(2) reduction of LaFeO_(3) perovskite

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Nano research 2024年第5期17卷 3733-3744页

作者： Chi Cao Jinshuo Li Yang Hu Lin Zhang Wensheng Yang State Key laboratory of inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China Engineering research Center for Nanomaterials Henan UniversityKaifeng 475004China

Three kinds of metal atoms with different valence electronic configurations,Bi(6s^(2)6p^(3)),Y(4d^(1)5s^(2)),and Ce(4f^(1)5d^(1)6s^(2)),were selected to investigate the effect of A-site(La^(3+))doping on electronic band structure,photoelectric properties,and photocatalytic performance of LaFeO_(3) *** was identified that the Bi doped LaFeO_(3) presented significantly improved photocatalytic activity towards the reduction of CO_(2),while the Y or Ce doped LaFeO_(3) displayed decreased photocatalytic activity compared to the pristine LaFeO_(3).It was revealed that doping of all the three metal atoms resulted in narrowed band gap and thus extended light absorption of LaFeO_(3) by lowering its conduction band minimum(CBM).The recombination rate and mobility of the charge carriers were represented by the relative effective mass(D)between holes and electrons for pristine and A-site doped LaFeO_(3).The doping of Bi resulted in increased D value,attributed to the Bi 6s electron states at the valence band maximum(VBM),and thus promoted separation and transfer of the charge carriers and improved photocatalytic activity of LaFeO_(3).In contrast,the doping of Ce resulted in significantly decreased D value,induced by the highly localized Ce 4f hole states at the CBM,and thus higher recombination rate of the charge carriers and decreased photocatalytic activity of LaFeO_(3).Furthermore,the Y doped LaFeO_(3) with a slightly decreased D value presented slightly increased recombination rate of the charge carriers and thus decreased photocatalytic *** a work provides new insights into the A-site doping in LaFeO_(3) perovskite,which should be helpful for optimizing the electronic band structure and activity of perovskite-type photocatalysts at atomic level.

关键词： A-site doping electronic band structure charge carrier behavior photocatalytic CO_(2)reduction perovskite-type photocatalytsts

The structure-directing role of heterologous seeds in the synthesis of zeolite

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Green Energy & Environment 2024年第5期9卷 792-801页

作者： Haoyang Zhang Binyu Wang Wenfu Yan State Key laboratory of inorganic Synthesis&Preparative chemistry College of ChemistryJilin UniversityChangchun130012China

Zeolites have been widely used as catalysts,ion-exchangers,and adsorbents in chemical industries,detergent industry,steel industry,glass industry,ceramic industry,medical and healthﬁeld,and environmentalﬁeld,and recently applied in energy ***-assisted synthesis is a very effective approach in promoting the crystallization of *** some cases,the target zeolite cannot be formed in the absence of seed *** homologous seed-assisted synthesis,the structure of the seed zeolite is the same to that of the target zeolite,while the structure of the seed zeolite is different to that of the target zeolite in the heterologous seed-assisted *** this review,we brieﬂy summarized the heterologous seed-assisted syntheses of zeolites and analyzed the structure-directing effect of heterologous seeds and surveyed the“common composite building units(CBUs)hypothesis”and the“common secondary building units(SBUs)hypothesis”.However,both hypotheses cannot explain all observations on the heterologous seed-assisted ***,we proposed that the formation of the target zeolite does need nuclei with the structure of target zeolite and the formation of the nuclei of the target zeolite can be promoted by either the undissolved seed crystals with the same CBUs or SBUs to the target zeolite or by the facilitated appropriate distribution of the speciﬁc building units due to the presence of the heterologous seed that does not have any common CBUs and SBUs with the target zeolite.

关键词： Zeolite Heterologous seed Synthesis Structure-directing effect

Engineering of efficient visible light photocatalysts:Ti_(1-x+y)Cu_(x)La_(y)O_(2)(x=0.03;y=0,0.005,0.01) compositions

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Journal of Rare Earths 2024年第3期42卷 497-505,I0003页

作者： S.M.Yakout A.M.Youssef inorganic chemistry Department National Research Centre(NRC)El Buhouth StDokkiCairo12622Egypt

In dye-photocatalysis, widening the wavelengths absorption range of catalysts as well as aborting the recombination of the photoexcited charge carriers(electrons-holes pairs) are of paramount *** the current study, we report the photocatalytic characteristics of four compositions composed of TiO_(2),Ti_(0.97)Cu_(0.03)O_(2), Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)powders for two harmful dyes(Congo red and methylene blue). The X-ray diffraction technique verified the configuration of mixed anatase and rutile phases in pure TiO_(2)and Ti_(0.97)Cu_(0.03)O_(2)powders while Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)powders possess anatase phase only. The changes of the band gap structure and dimensions of the unit cell volume of TiO_(2)confirm the substitution of Ti^(4+)sites by Cu^(2+)and La^(3+)ions. Remarkable widening of wavelengths absorption with formation of long absorption tails were found in TiO_(2)(3.13 e V) through insertion of La^(3+)plus Cu^(2+)ions. Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)samples exhibit a visible light band gap of 2.3 and 2.7 e V, respectively. Based on SEM images, incorporation of Cu^(2+)and La^(3+)ions influences the surface morphology of TiO_(2). The resulting Ti_(0.97)Cu_(0.03)O_(2), Ti_(0.965)Cu_(0.03)La_(0.005)O_(2)and Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)powders present enhanced photocatalytic activity towards Congo red dye degradation compared to pure one under natural solar spectrum. The best Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)catalyst exhibits superior photocatalytic activity of 96% for 10 ppm CR dye in 20 min as well as above average photocatalytic efficiency of 63% for 30 ppm CR dye in 120 min. As well, it showed acceptable photodegradation activity of 52% for 30 ppm MB solution in 140 min of sunlight irradiation. The heightened photodegradation efficiency of Ti_(0.96)Cu_(0.03)La_(0.01)O_(2)catalyst can be clarified in terms of higher ch

关键词： Semiconductor TiO_(2) Rare earths Congo red Methylene blue Solar spectrum Photodegradation

Regulation of Tumor Microenvironment Under Malignant Conditions:Application of nMOFs in Sonodynamic Therapy

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Chemical research in Chinese Universities 2024年第4期40卷 611-626页

作者： YANG Yilin YAN Fei SHI Zhan State Key laboratory of inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun130012P.R.China

In this review,we delve into the intricate regulation of the tumor microenvironment(TME)under malignant conditions and explore the transformative potential of nanoscale metal-organic frameworks(nMOFs)in the realm of sonodynamic therapy(SDT).The TME serves as a dynamic milieu influencing tumor progression and therapeutic response,presenting formidable challenges,such as hypoxia,acidity,excess hydrogen peroxide,high expression of glutathione,and *** the exceptional attributes of nMOFs,including their tunable structures and biocompatibility,holds immense promise for enhancing SDT efficacy and reshaping the TME *** integrating nMOFs with SDT,researchers aim to assemble multiple functionalities in a single platform that enhance tumor cell eradication while counteracting unfavorable TME conditions and immune *** potential of nMOFs to revolutionize tumor therapies by precisely targeting TME and overcoming therapeutic barriers is underscored by an in-depth analysis of recent breakthroughs in the use of nMOFs-based sonosensitizers to remodulate TME to amplify the efficacy of SDT.

关键词： Sonodynamic therapy Metal-organic framework Tumor microenvironment Modification of sonosensitizer

Facile synthesis of hierarchical NiO/NiFe_(2)O_(4) microsphere composite as efficient visible photocatalyst for 2,4-DCP degradation

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Rare Metals 2024年第4期43卷 1580-1588页

作者： Shabana Shaheen Shuai Xu Ji Bian Amir Zada Zi-Qing Zhang Yang Qu Li-Qiang Jing Key laboratory of Functional inorganic Materials chemistry(Ministry of Education) International Joint Research Center and Lab for Catalytic TechnologySchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin150080China Department of chemistry Abdul Wali Khan UniversityMardan23200Pakistan

It is highly desired to develop efficient photocatalysts with recycling property for practical application to degrade toxic ***,nanosheet-assembled NiFe_(2)O_(4)microspheres with commendable activity are successfully synthesized by a facile solvothermal reaction with NH4F as the modifier,and their photoactivities are further improved by coupling with NiO through an in situ growth *** optimized nickel oxide(NiO)/nickel ferrite(NiFe_(2)O_(4))microsphere composite(5NiO/NFO-4)exhibits a satisfactory photocatalytic activity for 2,4-dichlorophenol(2,4-DCP)degradation under visible-light irradiation,which is attributed to its wide visible-light response,well-designed hierarchical structure and enhanced charge transfer and separation by coupling NiO as a high-level energy platform to accept ***,it is found that the NiO/NiFe_(2)O_(4)microsphere photocatalysts can be easily collected and recycled owing to the distinctive magnetic *** work provides a feasible route to rational design visible-light-driven photocatalysts with high-activity for environmental remediation and purification with good recyclability.

关键词： NiFe_(2)O_(4) microspheres NiO/Fe_(2)O_(4) composite Charge separation Visible-light photocatalysis 2 4-Dichlorophenol degradation

Linear paired electrolysis of furfural to furoic acid at both anode and cathode in a multiple redox mediated system

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Green Energy & Environment 2024年第1期9卷 104-113页

作者： Xinxin Li Linchuan Cong Haibo Lin Fangbing Liu Xiangxue Fu Hai-Chao Xu Nan Lin State Key laboratory of inorganic Synthesis and Preparative chemistry Jilin UniversityChangchun 130012JilinChina State Key laboratory of Physical chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina

Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the ***,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedﬂow cell *** reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are *** the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efﬁciency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.

关键词： Multiple redox mediated system Linear paired electrolysis Furfural Furoic acid

Synergistic Ru/RuO_(2) heterojunctions stabilized by carbon coating as efficient and stable bifunctional electrocatalysts for acidic overall water splitting

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Nano research 2024年第8期17卷 6931-6939页

作者： Man Wu Yuying Fan Yang Huang Dongxu Wang Ying Xie Aiping Wu Chungui Tian Key laboratory of Functional inorganic Material chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080China

The development of highly active and stable acidic water oxidation electrocatalysts is of great significant for promoting the industrial application of proton exchange membrane ***-based catalysts have broad application prospects in acidic water oxidation,but their limitations in stability and activity hinder their further ***,a nitrogen-doped carbon(NC)coated porous Ru/RuO_(2) heterojunctional hollow sphere(Ru/RuO_(2)/NC)is designed as high-active and stable bifunctional electrocatalyst for acidic oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).In synthesis,the key is to use mesoporous polydopamine spheres as a template for forming hollow spheres,a source of NC coating and a reducing agent for forming Ru/RuO_(2) *** Ru/RuO_(2) heterojunction adjusts the electronic structure of Ru active sites,optimizing the adsorption of intermediate ***,the NC coating and the interaction between NC and Ru/RuO_(2) effectively prevent Ru from over-oxidation and *** porous hollow structure provides more exposed active sites and promotes mass ***,Ru/RuO_(2)/NC exhibits outstanding OER and HER performance with low overpotentials of 211 and 32 mV at 10 mA·cm^(−2),respectively,and shows excellent *** acid water splitting electrolyzer,based on the bifunctional Ru/RuO_(2)/NC,requires low cell voltages of 1.46 and 1.76 V at 10 and 100 mA·cm^(−2),respectively,with good stability for over 100 h operation,surpassing Pt/C||RuO_(2) and most of the reported catalysts.

关键词： hollow heterojunction bifunctional electrocatalysts oxygen evolution hydrogen evolution acidic water splitting

Single-atom Zn confined in hierarchical hollow microstructure as an acid/base-resistant microwave absorption materials

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Nano research 2024年第8期17卷 6785-6794页

作者： Yue Lou Jiao Li Xiaokun Li Zhenyu Zhu Zhan Shi Biao Xu School of chemistry and Chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China State Key laboratory of inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China

Developing acid/base-resistant and low-price microwave-absorbing materials with lighter weight is highly desired for practical applications in extreme ***,we demonstrate the successful synthesis of the N-doped porous carbon(NC)material with hierarchical pore structure by the spray pyrolysis *** large specific surface area(SBET=707.53 m^(2)·g^(−1))of materials enables multiple scattering of incident electromagnetic waves,and N doping greatly enhances the electrical conductivity of the ***,single-atom Zn can adjust the local electronic structure of adjacent sites such as carbon and nitrogen atoms,induce the center of polarization,and thus change the dielectric and electronic properties of the host *** porous carbon coating of single-atom Zn avoids the deterioration of electromagnetic parameters caused by the accumulation of magnetic particles under high-temperature *** the same time,they can also be used in various complex environments,such as acidic and basic ***,NC-1000,with high surface area,low density,and good chemical stability,obtained a minimum reflection loss(RLmin)of−50.5 dB and an effective absorption bandwidth(EAB)exceeding 5.1 GHz at the thickness of 1.9 *** soaking in the strong acid and base solution,the electromagnetic wave absorption performance of the material decreased by<15%.Widely available raw materials and a simple preparation scheme are expected to expedite industrial mass production for this novel type of materials.

关键词： hierarchical hollow microstructure microwave absorption metal-organic framework(MOF) impedance matching singleatom Zn acid/base-resistant

Progress and prospect of Pt-based catalysts for electrocatalytic hydrogen oxidation reactions

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Nano research 2024年第3期17卷 960-981页

作者： Xu Zhang Ying Xie Lei Wang Key laboratory of Functional inorganic Material chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080China

To achieve the goals of the peak carbon dioxide emissions and carbon neutral,the development and utilization of sustainable clean energy are extremely *** fuel cells are an important system for converting hydrogen energy into electrical ***,the slow hydrogen oxidation reaction(HOR)kinetics under alkaline conditions has limited its ***,elucidating the catalytic mechanism of HOR in acidic and alkaline media is of great significance for the construction of highly active and stable *** terms of practicality,Pt is still the primary choice for commercialization of fuel *** the above basis,we first introduced the hydrogen binding energy theory and bifunctional theory used to describe the HOR activity,as well as the pH *** that,the rational design strategies of Pt-based HOR catalysts were systematically classified and summarized from the perspective of activity *** addition,we further emphasized the importance of theoretical simulations and in situ characterization in revealing the HOR mechanism,which is crucial for the rational design of ***,the practical application of Pt-based HOR catalysts in fuel cells was also *** closing,the current challenges and future development directions of HOR catalysts were *** review will provide a deep understanding for exploring the mechanism of highly efficient HOR catalysts and the development of fuel cells.

关键词： Pt-based catalysts hydrogen oxidation reaction(HOR) electrocatalytic mechanism hydrogen binding energy theory bifunctional theory