Herein, we successfully regulated phosphorus vacancies in Co0.68Fe0.32P through Ar-plasma treatment. The Ar-plasma treated Co0.68Fe0.32P exhibits a delicate surface state where the surface Co and Fe ions show an unusual electron loss. The unique surface state enhances the oxygen evolving performance of the phosphide.
With precise control of reaction conditions, it is possible to accelerate the oxygen evolution kinetics through optimization of adsorption/dissociation equilibrium.
This work depicts the synthesis of controllable Pd nanoparticles decorated TiO2 nanowire arrays by electrospray technique. By varying the substrate temperature and volume of precursor solution, Pd/TiO2 hybrid structure with different sizes and deposition yield was precisely controlled. The highest photocurrent density of the Pd/TiO2 photoanode was 1.4 mA cm(-2) at 1.23 V vs. RHE, which was approximately 5 times higher than the pristine TiO2. The onset potential with a significant cathodic shift of 80 mV compared to the pristine TiO2 was also observed. To the best of our knowledge, the obtained photocurrent showed the optimal photocurrent density and high stability compared with previous reports. It is also found that the photoelectrochemical performance is closely related to the size and deposition quantity of Pd nanoparticles. According to the results, the enhanced PEC performance can be attributed to the Schottky junction, charge transfer and the enhancement about the separation efficiency of the photogenerated electrons and holes betweenTiO(2) and Pd NPs. This result demonstrated that this method may design a new and green strategy for synthesizing the well-defined morphologies, compositions, and sizes of the hybrid nanomaterial for photocatalytic hydrogen generation, photocatalytic CO2 reduction and photosynthesis of organic molecules. (C) 2019 Elsevier B.V. All rights reserved.
SmallVolume 15, Issue 29 1970153 Inside Front CoverFree Access ABO3-Type Perovskites: Unfolding BOB Bonds for an Enhanced ORR Performance in ABO3-Type Perovskites (Small 29/2019) Yu Sun, Yu Sun College of Chemistry, Jilin University, Changchun, 130012 P. R. ChinaSearch for more papers by this authorZhongyuan Liu, Zhongyuan Liu College of Chemistry, Jilin University, Changchun, 130012 P. R. ChinaSearch for more papers by this authorWei Zhang, Wei Zhang School of Materials Science and Engineering and Electron Microscopy Center, Jilin University, Changchun, 130012 P. R. ChinaSearch for more papers by this authorXuefeng Chu, Xuefeng Chu Jilin Provincial Key Laboratory of Architectural Electricity and Comprehensive Energy Saving, School of Electrical and Electronic Information Engineering, Jilin Jianzhu University, Changchun, 130118 P. R. ChinaSearch for more papers by this authorYingge Cong, Yingge Cong College of Chemistry, Jilin University, Changchun, 130012 P. R. ChinaSearch for more papers by this authorKeke Huang, Keke Huang College of Chemistry, Jilin University, Changchun, 130012 P. R. ChinaSearch for more papers by this authorShouhua Feng, Shouhua Feng College of Chemistry, Jilin University, Changchun, 130012 P. R. ChinaSearch for more papers by this author Yu Sun, Yu Sun College of Chemistry, Jilin University, Changchun, 130012 P. R. ChinaSearch for more papers by this authorZhongyuan Liu, Zhongyuan Liu College of Chemistry, Jilin University, Changchun, 130012 P. R. ChinaSearch for more papers by this authorWei Zhang, Wei Zhang School of Materials Science and Engineering and Electron Microscopy Center, Jilin University, Changchun, 130012 P. R. ChinaSearch for more papers by this authorXuefeng Chu, Xuefeng Chu Jilin Provincial Key Laboratory of Architectural Electricity and Comprehensive Energy Saving, School of Electrical and Electronic Information Engineering, Jilin Jianzhu University, Changchun, 130118 P. R. ChinaSearch for more papers by this authorYingge Cong, Yingge Cong College of Chemistry, Jilin University, Changchun, 130012 P. R. ChinaSearch for more papers by this authorKeke Huang, Keke Huang College of Chemistry, Jilin University, Changchun, 130012 P. R. ChinaSearch for more papers by this authorShouhua Feng, Shouhua Feng College of Chemistry, Jilin University, Changchun, 130012 P. R. ChinaSearch for more papers by this author First published: 19 July 2019 https://doi.org/10.1002/smll.201970153Citations: 1AboutPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShare Give accessShare full text accessShare full-text accessPlease review our Terms and Conditions of Use and check box below to share full-text version of article.I have read and accept the Wiley Online Library Terms and Conditions of UseShareable LinkUse the link below to share a full-text version of this article with your friends and colleagues. Learn more.Copy URL Share a linkShare onFacebookTwitterLinkedInRedditWechat Graphical Abstract With revealing the evolution of the B–O–B bond angle, Shouhua Feng and co-workers demonstrate in article number 1803513 the structure–effect relationship between B–O bond covalency and oxygen reduction reaction performance in ABO3-type perovskite oxides. This work is devoted to offering a fundamental theoretical and technical insight into precise regulation of electronic structure through design and construction of chemical bonds. Citing Literature Volume15, Issue29Special Issue: Advanced Materials for Green Chemistry and Renewable EnergyJuly 19, 20191970153 RelatedInformation
Charge transfer between LaCoO3 and La0.67Sr0.33MnO3 interface shortens the distance between O p-band center and the Fermi level.
The introduction of iron into Co3O4can induce a change in the electronic states of Co3+, which is an effective means to regulate the oxygen evolution reaction activity.
微信作为信息时代的主要产物,已经被大多数人普遍认可与使用.微信拉近了人与人之间的距离,也给人们的日常生活和工作带来了极大的便利.但对于高等院校而言,其肩负着教育学生的职责,而微信中一旦传播不良的信息,势必会影响大学生的健康成长,同时也影响大学生思想政治教育效果.基于此,分析在微信公众平台中有效进行大学生思想政治教育的方法,对于提高各大高校思想政治教育效果和引导大学生建立正确的价值取向意义重大.
大学生廉洁教育是贯穿在社会主义高等教育全过程的重要内容,它不仅仅是对学生个人人生信念、行为品性的塑造过程,更是培育良好社会风气,孕育公平正义的社会土壤,传承优秀传统文化的必然举措.历史和实践充分表明,将廉洁教育根植于大学生的日常教育中,从年轻时代就身体力行,崇尚廉洁,拒绝贪腐,系好人生的第一颗扣子,有利于职业和人生的双重塑造,有利于传承公正廉洁的优秀品格,从而有利于一代又一代形成"崇廉拒腐"的社会风气,为党的各项事业长期发展提供坚实保障.
Fe₂TiO₅ is recognized as a novel and promising photoanode material for solar water splitting. Here, nanostructured Fe₂TiO₅ was fabricated on a fluorine-doped tin oxide substrate by an electrospray deposition technique. We utilized surface Al³⁺ treatment and FeOOH modification to improve performance of the Fe₂TiO₅ photoanode. After this two-step enhancement, the photocurrent density of the final Fe₂TiO₅ photoanode is 0.52 mA cm–² at 1.23 VRHE which is 2.8 times that of the pristine one, and the onset potential is 200 mV lower than before. The enhanced performance can be attributed to a synergetic effect of surface Al³⁺ treatment and FeOOH modification, since the surface Al³⁺ treatment accelerates charge transport while the FeOOH layer improves catalytic activity. This strategy of surface modification provides an effective pathway for rational designing of original photoanodes with high practical performance.
>Interface effect is one of the central topics for decades[1–3].For inorganic composites,interface effect is mainly induced by interface stress[4]and interface charge transfer[4–6],in which interface charge transfer is a main factor affecting the chemical property of composites.A considerable amount of interface charge
The exsolution of noble metal nanoparticles (NPs) from perovskite usually requires high doping ratio of noble metal. Herein, we constructed a RuO2/LFRO composite by the exsolution of a low Ru-substituted A-site deficient perovskite, La0.9Fe0.92Ru0.08O3 (LFRO). In this process, pure Ru NPs are in situ exsolved from LFRO via a relatively low temperature heat treatment in 5% H2/Ar. Then the exsolved Ru NPs were oxidized to RuO2 for oxygen evolution reaction (OER) applications. The RuO2/LFRO composite achieved a high OER performance compared with the pristine LFRO, which is mainly originated from the generation of electrochemically active RuO2 NPs and the improvement of conductivity. In addition, the exsolution is a reversible process that the exsolved Ru NPs can disappear into the perovskite lattice at 550 °C in air. Our work thereof demonstrates an effective strategy to minimize the dosage of precious metals for catalytic applications in different fields.
High Bi-ratio ternary sulfides have been recently reported as superior thermoelectric materials. However, the synthesis of high Bi-ratio Cu-Bi-S nanocrystal remains a challenge. Reported here are the synthesis and characterization of three-phase Cu-Bi-S nanocrystals with the nominal chemical formulae of Cu1.57 Bi4.57 S8 , Cu2.93 Bi4.89 S9 and Cu3 BiS3 . The samples were prepared using a Bi2 S3 precursor by varying the amount and type of Cu2-x S (i. e. Cu2 S or Cu7.2 S4 ) reactants. TEM images reveal that two new samples crystalized having nanorod morphology with radii of approximately 50 nm and lengths of 200 nm. XPS results indicate that the valence states of Bi in both the two new phases are +3 with viable oxidation states for Cu. UV-Vis-NIR absorption spectroscopy reveals that narrow direct bandgaps are 1.12 and 1.27 eV for Cu1.57 Bi4.57 S8 and Cu2.93 Bi4.89 S9 , respectively. Besides, this method could also be applied to synthesize the Cu3 BiS3 phase with a new nanoplate morphology. The as-synthesized Cu-Bi-S samples show Cu/Bi ratio-dependent photoresponsive properties. This study not only reports the structure and bandgap of two ternary sulfides, which have only been discovered in the mineral previously, but also provides an efficient method for synthesizing Bi-rich ternary chalcogenide nanocrystals.
Metal oxide hollow structures with large surface area, low density, and high loading capacity have received great attention for energy‐related applications. Acting as oxygen‐related catalysts, hollow‐structured transition metal oxides offer low overpotential, fast reaction rate, and excellent stability. Herein, recent progress in the oxygen‐related catalysis (e.g., oxygen evolution reaction (OER), oxygen reduction reaction (ORR), and metal–air batteries) of hollow‐structured transition metal oxides is discussed. Through a comprehensive outline of hollow‐structured spinels, perovskites, rutiles, etc., a rational design strategy is provided for an enhanced oxygen‐related catalysis performance from the viewpoint of crystal structures. Urgent challenges and further research directions are presented for hollow‐structured transition metal oxides toward excellent oxygen‐related catalysis.
Cation segregation of perovskite oxide is crucial to develop high-performance catalysts. Herein, we achieved the exsolution of α-Fe2O3 from parent La0.85FeO3-δ by a simple heat treatment. Compared to α-Fe2O3 and La0.85FeO3-δ, α-Fe2O3-LaFeO3- x achieved a significant improvement of lithium-oxygen battery performance in terms of discharge specific capacity and cycling stability. The promotion can be attributed to the interaction between α-Fe2O3 and LaFeO3- x. During the cycling test, α-Fe2O3-LaFeO3- x can be stably cycled for 108 cycles at a limited discharge capacity of 500 mAh g-1 at a current density of 100 mA g-1, which is remarkably longer than those of La0.85FeO3-δ (51 cycles), α-Fe2O3 (21 cycles), and mechanical mixing of LaFeO3 and α-Fe2O3 (26 cycles). In general, these results suggest a promising method to develop efficient lithium-oxygen battery catalysts via segregation.
Electrical conductivity between substrate and catalyst is a key factor restricting the OER (oxygen evolution reaction) catalytic activity of transition metal oxides. Herein we report a facile and direct route for synthesizing spinel NiCo2O4 nanostructure on conductive substrates by electrospray technique. By simply altering the substrate temperature, film thickness and voltage, NiCo2O4 with different morphology and electrocatalytic performance was obtained. The optimal performance showed a low overpotential of 375 mV at 10 mA/cm(2) and an excellent stability over 15 h. This work proved that electrospray technology is an effective strategy to fabricate the binder-free catalysts with high activity and stability for OER. (C) 2018 Elsevier B.V. All rights reserved.
Anionic redox chemistry is becoming increasingly important in explaining the intristic catalytic behavior in transition-metal oxides and improving catalytic activity. However, it is a great challenge to activate lattice oxygen in noble-metal-free perovskites for obtaining active peroxide species. Here, we take La0.4Sr0.6CoO3-δ as a model catalyst and develop an anionic redox activity regulation method to activate lattice oxygen by tuning charge transfer between Co4+ and O2-. Advanced XAS and XPS demonstrate that our method can effectively decrease electron density of surface oxygen sites (O2-) to form more reactive oxygen species (O2- x), which reduces the activation energy barriers of molecular O2 and leads to a very high CO catalytic activity. The revealing of the activation mechanism for surface oxygen sites in perovskites in this work opens up a new avenue to design efficient solid catalysts. Furthermore, we also establish a correlation between anionic redox chemistry and CO catalytic activity.
Nonenzymatic dehydration reactions of decanoic acid with glycerol has been reported to occur under mimicked prebiotic conditions at near neutral pH, yielding more evolved membrane precursor compound glyceryl decanoates. Two isomers of glyceryl monodecanoate were the main products after the condensation reactions, and the yield of glyceryl monodecanoates could be increased to 4. 7% with temperature rising to 90 degrees C. Vesicles were observed when the mixture after reactions was rehydrated. Experiments demonstrate that trace glyceryl decanoates produced in the mixture play a great role in robust self-assembly process, it is the existence of such lipid products that makes a lower critical vesicle concentration. Meanwhile, organic compounds have been encapsulated during the self-assembly of vesicles, so membranous structures provid a place for organic compounds to exist stably. The dehydration reactions at near neutral pH, followed by rehydration, are suitable for increasing protocell membrane stability to environment. It implies that the condensation reaction is plausible for yielding more complex amphiphiles and the appearance of membrane structures on the early earth.
Amorphous materials exhibit distinct physical and chemical properties compared to crystalline or quasi-crystalline phases, because of their unique atomic arrangements of short-range order but long-range disorder. Designing a nanocomposite that contains both crystalline and amorphous phases is a valid approach to fully exploit the effects of each component. In this work, a nanocomposite consisting of crystalline Ag2S nanoparticles embedded in an amorphous Cu2S matrix (Ag2S/a-Cu2S) is synthesized by a facile one-pot solvothermal method. This process is achieved by diffusing silver into crystalline Cu2S. The silver is able to diffuse into Cu2S and form crystalline Ag2S nanoparticles inside them, while the crystalline Cu2S is converted into an amorphous phase owing to the silver diffusion. Furthermore, the introduction of nanoscale Ag2S particles into Cu2S improve electrical conductivity. This design of amorphous matrix containing nanocrystalline particles may open up new strategies for the transition from crystalline to amorphous phases of semiconductors.
Mn4CaO5 cluster in green plant is considered as the ideal structure for water oxidation catalysis. However, this structure is difficult to be constructed in heterogeneous catalyst because of its distorted spatial structure and unique electronic state. Herein, we report the synthesis of two-dimensional biomimetic Ca-Mn-O catalyst with Mn4CaO5 clusterlike structure through ultrasonic-assisted reduction treatment toward Ca-birnessite. The synergistic effect between ultrasonic and reduction successfully reduced the Mn oxidation state in Ca-birnessite without breaking the structure of MnO2 monolayers, forming a regular two-dimensional structure with Mn4CaO5 cubanelike structure unit for the first time. The biomimetic catalyst shows a superior water oxidation activity (turnover frequency = 3.43 s-1), which is the best in manganese-based heterogeneous catalyst to date. This work provides a new strategy for the precise synthesis of specific structure and exhibits a great prospect of biomimic in heterogeneous catalyst.
大学生社会实践活动是学生走出校门、接触社会、了解国情、学以致用的重要机会,是使理论与实践相互结合、学生与广大群众相互联系的良好形式,是大学生投身社会建设、向群众学习、培养锻炼才干的重要渠道;是提升思想觉悟、增强大学生服务社会意识,促进大学生健康成长的有效途径.对高校家庭经济困难的学生更具有重要意义,高校应采取有效措施引导其积极参与社会实践活动,更好地实现育人的作用.