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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

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Effect of Rosmarinus officinalis and Origanum majorana extracts on stability of sunflower oil during storage and repeated heating

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Oil Crop Science 2024年第1期9卷 29-37页

作者： Ali Sahunie department of analytical and Food chemistry Tishreen UniversityLattakiaSyria

Both rosemary(Rosmarinus officinalis)and marjoram(Origanum majorana)are abundant in phenolic compounds,exhibiting exceptional antioxidant *** study aims to assess the impact of rosemary and marjoram extracts on the stability of sunflower oil during storage and repeated *** oil supplemented with herbal extracts or butylated hydroxytoluene(BHA)at a concentration of 200 ppm was stored for six months under light and dark conditions at room *** value(PV),p-anisidine value(An-V),and total oxidation(TOTOX)value were measured to monitor lipid oxidation progression.A significant difference(P<0.05)was observed between light and dark storage for all studied samples regarding oxidation *** ethanolic extract of rosemary exhibited higher antioxidant activity compared to BHA and other ***,sunflower oil supplemented with the ethanolic extract of rosemary underwent weekly treatment at 100℃for 30 min over four consecutive *** all oxidation indicators increased during repeated heating,the addition of rosemary and marjoram extracts as well as BHA significantly reduced these *** findings demonstrate that both rosemary extracts and marjoram extracts can serve as natural antioxidants in edible oils.

关键词： Phenolic compounds BHA Marjoram extract Rosemary extract Sunflower oil

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CO oxidation under lean and stoichiometric conditions over ceriazirconia with very low metal contents(Cu,Co,Ag and Pt)

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Journal of Rare Earths 2024年第9期42卷 1669-1681页

作者： J.C.Martínez-Munuera M.P.Yeste A.García-García MCMA Group Department of Inorganic Chemistry and Institute of MaterialsUniversity of Alicante Solid chemistry and Catalysis Group Department of Materials ScienceMetallurgic Engineering and Inorganic ChemistryInstitute of Electronic Microscopy and Materials ResearchUniversity of Cádiz

In this work,several ceria-zirconia based catalysts with very lo w（and equimolar） metal contents were prepared,characterised and tested for the CO oxidatio n reaction（under lean and stoichiometric conditions）,trying to emulate those conditions found in a diesel oxidation catalyst（DOC） system from a diesel engine and those encountered under gasoline exhaust（λ=1）.The metals chosen are Cu,Co,Ag and Pt（as a reliable benchmark）.The results reveal enormous differences among reducibility and catalytic activity despite quite similar structural and textural properties of the catalysts,showing differences among dispersion（Ag-catalyst seems to present a low level of dispersion）.This catalyst seems to be characterised,as well,by a strong electronic interaction between Ce and Ag centres which is suggested to yield an improved reducibility under H2-TPR ***,the order in catalytic activity（Cu>Ag>Co≈Pt>>support） seems not to follow the order found in reducibility and the Cu-catalyst seems to be the most active independently on the reaction conditions,yielding nearly overlapped CO oxidation catalytic *** restingly,a stro ng correlation between the catalytic activity under the two conditions tested and the OSC values of the Ce0.8Zr0.2O2-supported metal catalysts is ***,OSC parameter measured at 150℃ can be used as a relevant descriptor to evaluate the CO oxidation activity at low and medium conversions for the investigated catalysts,much better than the H2-TPR measurements.

关键词： CO oxidation Low metal content Ceria-zirconia Copper species OSC parameter Rare earths

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Geometric and defects engineering collaboration for enhanced cascade enzymatic nanoreactors

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Nano Research 2024年第4期17卷 2451-2461页

作者： Zhichao Yu Ruijin Zeng Hexiang Gong Yuan Gao Shuyun Chen Yunsen Wang Dianping Tang Key Laboratory for analytical Science of Food Safety and Biology(MOE&Fujian Province) Department of ChemistryFuzhou UniversityFuzhou 350108China

Highly evolved multi-enzyme cascade catalytic reactions in organisms facilitate rapid transfer of substrates and efficient conversion of intermediates in the catalytic unit,thus rationalizing their efficient *** this study,pore-ordered mesoporous single-atom(Fe)nitrogen-doped carbon nanoreactors(Mp-Fe-CN)were designed,in which a reasonable pore size was designed as a natural enzyme trap coupled to a simulated enzyme center.A polarity-mediated strategy was developed to obtain atomically dispersed nanoporous substrates,with the finding that polarity-guided engineering of the nitrogen-ligand environment and vacancy cluster defects clearly affects nanoporous activity,accompanied by appreciable mesoporous pore size *** active center and distal N atom coordination of Fe-N_(4) affect the catalytic process of the nanozyme exposed by density functional theory(DFT),determining the contribution of hybridized orbitals to electron transfer and the decisive step.A cascade nanoreactor-based domain-limited sarcosine oxidase developed for non-invasive monitoring of sarcosine levels in urine for evaluation of potential prostate carcinogenesis as a proof of *** on the design of surface mesoporous channels of nanocatalytic units,a bridge was built for the interaction between nanozymes and natural enzymes to achieve cascade nanocatalysis of natural enzymatic products.

关键词： nanozyme single-atom catalyst bioreactor cascade catalysis non-Invasive sensing

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Rational modulation of electronic structure in PtAuCuNi alloys boosts efficient electrocatalytic ethanol oxidation assisted with energy-saving hydrogen evolution

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Journal of Energy chemistry 2024年第6期93卷 557-567,I0014页

作者： Hu Yao Yinan Zheng Xin Yu Songjie Hu Baolian Su Xiaohui Guo Key Lab of Synthetic and Natural Functional Molecule chemistry of Ministry of Education The College of Chemistry and Materials ScienceNorthwest UniversityXi’an 710069ShaanxiChina department of inorganic chemistry University of NamurBruxellesB-5000 NamurBelgium

Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient ***,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.215 V at 10 mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 10 mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and *** electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and ***,in the ethanol-assisted overall water splitting(E-OWS),a current density of 10 mA cm^(-2)was achieved at 0.28 ***,an advanced acid-base self-powered system(A-Bsps)that can achieve a self-powered voltage of 0.59 V was ***,the self-driven hydrogen production with zero external power supply was realized by integrating A-Bsps with the E-OWS *** interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields.

关键词： Pt-based alloy Electronic structure Ethanol oxidation Self-powered system Overall water splitting

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Hydrochar and synthetic natural gas co-production for a full circular economy implementation via hydrothermal carbonization and methanation:An economic approach

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Journal of Environmental Sciences 2024年第6期140卷 69-78页

作者： Judith González-Arias Guillermo Torres-Sempere Miriam González-Castaño Francisco MBaena-Moreno Tomás RReina inorganic chemistry department and Materials Sciences Institute University of Seville-CSICSevilleSpain Materials Sciences Institute(ICMSE) CSIC-University of SevilleSevilleSpain department of chemistry and Chemical Engineering Chalmers University of TechnologyGothenburgSE 41296Sweden

Herein we study the economic performance of hydrochar and synthetic natural gas coproduction from olive tree *** process entails a combination of hydrothermal carbonization and *** a previous work,we evidenced that standalone hydrochar production via HTC results ***,we propose a step forward on the process design by implementing a methanation,adding value to the gas effluent in an attempt to boost the overall process techno-economic *** different plant capacities were analyzed(312.5,625 and 1250 kg/hr).The baseline scenarios showed that,under the current circumstances,our circular economy strategy in *** analysis of the revenues shows that hydrochar selling price have a high impact on NPV and subsidies for renewable coal production could help to boost the profitability of the *** the contrary,the analysis for natural gas prices reveals that prices 8 times higher than the current ones in Spain must be achieved to reach *** seems unlikely even under the presence of a strong subsidy *** costs analysis suggests that a remarkable electricity cost reduction or electricity consumption of the HTC stage could be a potential strategy to reach profitability ***,significant reduction of green hydrogen production costs is deemed instrumental to improve the economic performance of the *** results show the formidable techno-economic challenge that our society faces in the path towards circular economy societies.

关键词： Hydrothermal carbonization CO_(2)waste valorization Methanation Profitability analysis

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Simultaneous improving luminescence intensity and stability of CsPbBr_(3):SCN−@Eu/Zr-Uio-66-NH_(2)with tunable emissions from blue to green and applications in indoor photovoltaics

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Nano Research 2024年第8期17卷 6879-6887页

作者： Minze Li Yao Sun Honglai Lu Peifen Zhu Ruihong Wang Guofeng Wang Key Laboratory of Functional inorganic Material chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China department of Electrical Engineering and Computer Science University of MissouriColumbiaMO 65211USA

The construction of stable and efficient materials that emit blue and green light remains a *** the blue light materials reported,metal-organic framework(MOF)materials are rarely reported as blue phosphors due to their weak luminescence *** on the construction of CsPbBr_(3)@MOF(CPB@MOF),an innovative idea was proposed to simultaneously enhance the green luminescence of CPB and the blue luminescence of MOF through the interaction between CPB and MOF for the first *** expected,the blue luminescence from CPB:7%SCN−@0.5%MOF:Eu as well as the green luminescence from 5%CPB:7%SCN−@MOF:Eu was sufficient to construct high-performance light-emitting diode(LED)devices and further excite solar cells to generate stable photoelectric *** white LED(WLED)device with excellent color quality(color rendering index(CRI)=96.2)and correlated color temperature(CCT=9688 K)can be constructed by using the obtained blue-emitting CPB:7%SCN-@0.5%MOF:Eu,green-emitting 5%CPB:7%SCN−@MOF:Eu,and red-emitting PPB:30%Mn^(2+).The density functional theory(DFT)theoretical calculation results indicate that the p orbital of Pb plays the major role in the conduction band,and the p orbital of Br plays the major role in the valance band of CPB and CPB:SCN−.While the p orbital of O plays the major role in both the conduction band and valance band of *** heat capacity of CPB and CPB:SCN−separately reaches the Dulong–Petit limit at 200 and 400 K,indicating that the thermal stability of CsPbBr_(3)increases after SCN−doping.

关键词： CsPbBr_(3):SCN−@Uio-66-NH_(2)composites luminescence stability white light-emitting diodes(WLEDs) indoor photovoltaics density functional theory(DFT)calculation

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Carbon Monoxide as C1 Building Block in Fine Chemical Synthesis

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Chinese Journal of chemistry 2024年第2期42卷 199-221页

作者： Rui M.B.Carrilho Mario J.F.Calvete Gabor Mikle Laszlo Kollar Mariette M.Pereira University of Coimbra Coimbra Chemistry CentreDepartment of ChemistryRua Larga3004-535 CoimbraPortugal department of General and inorganic chemistry and ELKH-PTE Research Groupfor Selective Chemical Syntheses University of PecsIfjusag utja 6H-7624 PecsHungary

Carbon monoxide(CO)has become one of the most relevant and versatile renewable C1 building blocks for chemical synthesis,especially in the fine chemicals industry,due to the development of efficient and selective catalysts for its *** this review,we present a comprehensive critical analysis of the last 10 years literature on the use of CO as a renewable feedstock for fine chemicals *** review is organized by type of catalytic reaction,namely alkene and alkyne carbonylation,hydroformylation,carbonylation of aryl halides,carbonylative cross-coupling and C-H *** examples of the synthesis of relevant building blocks and/or known pharmaceuticals are *** is placed on examples of utilizing CO as the C1 building block in one or more catalytic *** catalyst used and the reaction conditions are consistently presented throughout all of the examples.

关键词： Carbon monoxide Fine chemicals Carbonylation Hydroformylation C-H functionalization

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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

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Deciphering the controlling factors for phase transitions in zeolitic imidazolate frameworks

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National Science Review 2024年第4期11卷 151-163页

作者： Tao Du Shanwu Li Sudheer Ganisetti Mathieu Bauchy Yuanzheng Yue Morten M.Smedskjaer department of chemistry and Bioscience Aalborg University department of Mechanical Engineering-Engineering Mechanics Michigan Technological University Physics of Amo Rphous and inorganic Solids Laboratory(PARISlab) Department of Civil and Environmental EngineeringUniversity of CaliforniaLos Angeles

Zeolitic imidazolate frameworks（ZIFs） feature complex phase transitions, including polymorphism,melting, vitrification, and polyamorphism. Experimentally probing their structural evolution during transitions involving amorphous phases is a significant challenge, especially at the medium-range length scale. To overcome this challenge, here we first train a deep learning-based force field to identify the structural characteristics of both crystalline and non-crystalline ZIF phases. This allows us to reproduce the structural evolution trend during the melting of crystals and formation of ZIF glasses at various length scales with an accuracy comparable to that of ab initio molecular dynamics, yet at a much lower computational cost. Based on this approach, we propose a new structural descriptor, namely, the ring orientation index, to capture the propensity for crystallization of ZIF-4(Zn（Im）2, Im = C3H3N2-) glasses, as well as for the formation of ZIF-zni(Zn（Im）2) out of the high-density amorphous phase. This crystal formation process is a result of the reorientation of imidazole rings by sacrificing the order of the structure around the zinc-centered tetrahedra. The outcomes of this work are useful for studying phase transitions in other metal-organic frameworks（MOFs） and may thus guide the development of MOF glasses.

关键词： metal-organic frameworks phase transitions melting glass formation transferable deep learning force field ring orientation

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