Reconstructed Water Oxidation Electrocatalysts: The Impact of Surface Dynamics on Intrinsic Activities

Electroreduction of small molecules such as H₂O, CO₂, and N₂ for producing clean fuels or valuable chemicals provides a sustainable approach to meet the increasing global energy demands and to alleviate the concern on climate change resulting from fossil fuel consumption. On the path to implement this purpose, however, several scientific hurdles remain, one of which is the low energy efficiency due to the sluggish kinetics of the paired oxygen evolution reaction (OER). In response, it is highly desirable to synthesize high-performance and cost-effective OER electrocatalysts. Recent advances have witnessed surface reconstruction engineering as a salient tool to significantly improve the catalytic performance of OER electrocatalysts. In this review, recent progress on the reconstructed OER electrocatalysts and future opportunities are discussed. A brief introduction of the fundamentals of OER and the experimental approaches for generating and characterizing the reconstructed active sites in OER nanocatalysts are given first, followed by an expanded discussion of recent advances on the reconstructed OER electrocatalysts with improved activities, with a particular emphasis on understanding the correlation between surface dynamics and activities. Finally, a prospect for clean future energy communities harnessing surface reconstruction-promoted electrochemical water oxidation will be provided.     

Substrate temperature-controlled precursor reaction mechanism of PEALD-deposited MoOx thin films

Journal of Materials Science - Molybdenum oxide (MoOx) films had been grown by using plasma-enhanced atomic layer deposition (PEALD) with Mo(CO)6 precursor and O2 plasma reactant in a substrate...     

Advances in statistical mechanics of rock masses and its engineering applications

To efficiently link the continuum mechanics for rocks with the structural statistics of rock masses,a theoretical and methodological system called the statistical mechanics of rock masses(SMRM)was developed in the past three decades.In SMRM,equivalent continuum models of stressestrain relationship,strength and failure probability for jointed rock masses were established,which were based on the geometric probability models characterising the rock mass structure.This follows the statistical physics,the continuum mechanics,the fracture mechanics and the weakest link hypothesis.A general constitutive model and complete stressestrain models under compressive and shear conditions were also developed as the derivatives of the SMRM theory.An SMRM calculation system was then developed to provide fast and precise solutions for parameter estimations of rock masses,such as full-direction rock quality designation(RQD),elastic modulus,Coulomb compressive strength,rock mass quality rating,and Poisson’s ratio and shear strength.The constitutive equations involved in SMRM were integrated into a FLAC3D based numerical module to apply for engineering rock masses.It is also capable of analysing the complete deformation of rock masses and active reinforcement of engineering rock masses.Examples of engineering applications of SMRM were presented,including a rock mass at QBT hydropower station in northwestern China,a dam slope of Zongo II hydropower station in D.R.Congo,an open-pit mine in Dexing,China,an underground powerhouse of Jinping I hydropower station in southwestern China,and a typical circular tunnel in Lanzhou-Chongqing railway,China.These applications verified the reliability of the SMRM and demonstrated its applicability to broad engineering issues associated with jointed rock masses.     

Evolution of Local Structural Ordering and Chemical Distribution upon Delithiation of a Rock Salt–Structured Li1.3Ta0.3Mn0.4O2 Cathode

Lithium‐rich disordered rock‐salt oxides have attracted great interest owing to their promising performance as Li‐ion battery cathodes. While experimental and theoretical efforts are critical in advancing this class of materials, a fundamental understanding of key property changes upon Li extraction is largely missing. In the present study, single‐crystal synthesis of a new disordered rock‐salt cathode material, Li_1.3Ta_0.3Mn_0.4O₂ (LTMO), and its use as a model compound to investigate Li concentration–driven evolution of local cationic ordering, charge compensation, and chemical distribution are reported. Through the combined use of 2D and 3D X‐ray nanotomography, it is shown that Li removal accompanied by oxygen oxidation is correlated with the development of morphological defects such as particle cracking. Chemical heterogeneity, quantified by subparticle level distribution of Mn valence state, is minimal during Mn redox, which drastically increases upon the formation of cracks during oxygen redox. Density functional theory and bond valence sum mismatch calculations reveal the presence of local short‐range ordering in the pristine oxide, which gradually disappears along with the extraction of Li. The study suggests that with cycling the transformation into true cation–disordered state can be expected, which likely impacts the voltage profile and obtainable energy density of the oxide cathodes.     

基于数据拼接的金刚石刀具刃口三维形貌表征技术

原子力显微镜(AFM)是获取金刚石刀具刃口纳米级三维形貌的重要手段,但其存在测量范围小,难以表征参与切削区域整段刃口形貌特征的问题。采用基于迭代最近点法的刃口AFM测量数据拼接算法,获得了由多组数据拼接得到的刃口纳米级三维形貌,并进行了切削实验验证。实验结果表明,采用的数据拼接方法可较好地用于表征刀具刃口三维形貌。     

石墨烯改性涂层防护性能研究

为减少团聚，提高石墨烯在涂层中的分散性，研究采用纳米分散技术预先制备了石墨烯分散液，再将其分散至环氧树脂中获得石墨烯改性复合涂层。通过对石墨烯含量为 0、0.3%、0.6%的复合涂层进行盐水浸泡、盐雾、阴极剥离实验及电化学性能测试，证明石墨烯的加入显著增强了涂层的防护性能。石墨烯复合涂层在 3.5%盐水中浸泡 1 008 h后，涂层低频阻抗仍大于 106 Ω·cm²比未添加石墨烯的涂层提高了 3个数量级，且盐雾实验 6 000 h后涂层表面仍保持完好；含 0.6%石墨烯，的涂层耐蚀行为劣于石墨烯含量为 0.3%的涂层。     

负载型Pt-Fe/SiO_2催化剂催化环己烷一步氧化制己二酸

己二酸是合成尼龙-66和尼龙-46纤维的重要原料,并进一步用于生产许多重要的化工产品。工业上的己二酸多采用以硝酸为氧化剂的两步法合成,该工艺不仅工艺复杂,而且对设备有腐蚀作用,还会释放大量的温室气体N_2O。本文以负载型Pt/SiO_2、Fe/SiO_2和Pt-Fe/SiO_2为催化剂,采用过氧化氢和氧气为氧源,研究了环己烷一步氧化制己二酸的绿色合成路线。对催化剂进行ICP、BET比表面积、XRD、TEM等表征,结果表明,Pt-Fe/SiO_2催化剂中不存在与Pt或Fe对应的衍射峰。在最佳反应条件下,用高压釜进行了催化剂性能评价,结果表明,Pt-Fe/SiO_2催化活性略优于Pt/SiO_2和Fe/SiO_2。在环己烷转化率为28%的情况下,己二酸选择性达到33%。     

拉深筋对板材变形特征和力学性能的影响研究

采用实验方法将金属板材拉过不同尺寸的拉深筋镶块，分析了拉深筋高度、圆角半径以及过筋次数对板材变形特征的影响规律，研究了过筋产生的预应变对板材后续力学性能的影响规律。结果表明：板材流过拉深筋后，流动方向上发生均匀的拉伸变形；过筋产生的预应变随着拉深筋高度增大而增大，随着圆角半径增大而减小，随着过筋次数增加而近似线性增大；预应变越大，材料后续屈服强度和抗拉强度越高，但后续延伸率越小，总延伸率随着预应变增大表现出先减小后增大的趋势。     

Tribological and corrosion behaviors of fluorocarbon coating reinforced with sodium iron titanate platelets and whiskers

A series of sodium iron titanate (NFTO)–fluorocarbon composite coatings have been prepared with the liquid-phase blending method. The effects of two types of NFTO, NFTO platelets, and NFTO whiskers, on the tribological and corrosion behaviors of the composite coatings, are systematically studied. The results show that the addition of NFTO can significantly enhance the friction-reducing and wear resistance performances of the fluorocarbon coating. Under dry sliding, the minimum specific wear rate is 1.67 × 10⁻⁴ mm³/Nm for the platelet-filled composite coatings and 1.15 × 10⁻⁴ mm³/Nm for the whisker-filled composite coatings, respectively, showing a decrease of 83.5 and 88.6% than that of pure coating. Under a simulated seawater environment, the minimum specific wear rate is 5.44 × 10⁻⁵ mm³/Nm for the platelet-filled composite coatings and 0.84 × 10⁻⁵ mm³/Nm for the whisker-filled composite coatings, respectively, showing a decrease of 90.5 and 98.5% than that of pure coating. The morphologies of worn surfaces, wear debris, and transfer films are analyzed, and the corresponding wear resistance mechanisms are discussed. The electrochemical impedance spectroscopy certifies a remarkably improved corrosion resistance of the composite coatings which have been immersed in 3.5 wt % NaCl solution for 30 days. The composite coating reinforced with 7.5 wt % platelets shows the highest resistance of 256.3 × 10⁶ Ω·cm², approximately two orders of magnitude higher than that of pure coating. © 2020 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020 , 137, 48936.