Reaction environment self-modification on low-coordination Ni2+ octahedra atomic interface for superior electrocatalytic overall water splitting

Large scale synthesis of high-efficiency bifunctional electrocatalyst based on cost-effective and earth-abundant transition metal for overall water splitting in the alkaline environment is indispensable for renewable energy conversion. In this regard, meticulous design of active sites and probing their catalytic mechanism on both cathode and anode with different reaction environment at molecular-scale are vitally necessary. Herein, a coordination environment inheriting strategy is presented for designing low-coordination Ni²⁺ octahedra (L-Ni-8) atomic interface at a high concentration (4.6 at.%). Advanced spectroscopic techniques and theoretical calculations reveal that the self-matching electron delocalization and localization state at L-Ni-8 atomic interface enable an ideal reaction environment at both cathode and anode. To improve the efficiency of using the self-modification reaction environment at L-Ni-8, all of the structural features, including high atom economy, mass transfer, and electron transfer, are integrated together from atomic-scale to macro-scale. At high current density of 500 mA/cm², the samples synthesized at gram-scale can deliver low hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) overpotentials of 262 and 348 mV, respectively.

     

Superconvergence analysis of nonconforming finite element method for time-fractional nonlinear parabolic equations on anisotropic meshes

In this paper, we prove a novel result of the consistency error estimate with order $O\left(h^2\right)$ for $E{Q}_1^{rot}$ element (see Lemma 2) on anisotropic meshes. Then, a linearized fully discrete Galerkin finite element method (FEM) is studied for the time-fractional nonlinear parabolic problems, and the superclose and superconvergent estimates of order $O(\tau +h^2)$ in broken $H^1$-norm on anisotropic meshes are derived by using the proved character of $E{Q}_1^{rot}$ element, which improve the results in the existing literature. Numerical results are provided to confirm the theoretical analysis.     

Chemical bond characteristics and infrared reflectivity spectrum of a novel microwave dielectric ceramic CaIn2O4 with near-zero τf

Orthorhombic-structured CaIn₂O₄ ceramics with a space group Pca2₁ were synthesized via a solid-state reaction method. A high relative density (95.6 %) and excellent microwave dielectric properties (ε_r ～11.28, Qf = 74,200 GHz, τ_f ～ ?4.6 ppm/°C) were obtained when the ceramics were sintered at 1375 °C for 6 h. The dielectric properties were investigated on the basis of the Phillips–Van Vechten–Levine chemical bond theory. Results indicated that the dielectric properties were mainly determined by the InO bonds in the CaIn₂O₄ ceramics. These bonds contributed more (74.65 %) to the dielectric constant than the CaO bonds (25.35 %). Furthermore, the intrinsic dielectric properties of the CaIn₂O₄ ceramics were investigated via infrared reflectivity spectroscopy. The extrapolated microwave dielectric properties were ε_r ～10.12 and Qf = 112,200 GHz. Results indicated that ion polarization is the main contributor to the dielectric constant in microwave frequency ranges.     

Effects of Sr2+ substitution on the crystal structure,Raman spectra,bond valence and microwave dielectric properties of Ba3-xSrx(VO4)2 solid solutions

The effects of Sr²⁺ substitution for Ba²⁺ on microwave dielectric properties and crystal structure of Ba_3-xSr_x(VO₄)₂ (0 ≤ x ≤ 3, BSVO) solid solution were investigated. Such Sr²⁺ substitution contributes to significant reduction in sintering temperature from 1400 °C to 1150 °C. Both permittivity (∑_r) and quality factor (Q × f) values decreased with increasing x value, which was determined to be related with the descending values of average polarizability and packing fraction, whereas the increase in τ_f value was explained by the decreased average VO bond length, A-site bond valence. BSVO ceramics possessed encouraging dielectric performances with ∑_r = 12.2–15.6 ± 0.1, Q × f = 44,340 - 62,000 ± 800 GHz, and τ_f = 24.5–64.5 ± 0.2 ppm/°C. Low-temperature sintering was manipulated by adding B₂O₃ as sintering additive for the representative Sr₃V₂O₈ (SVO) ceramic and only 1 wt.% B₂O₃ addition successfully contributed to a 21.7% decrease in sintering temperature to 900 °C, showing good chemical compatibility with silver electrodes, which render BSVO series and SVO ceramics potential candidates in multilayer electronic devices fabrication.     

Plasmonic coupling-enhanced in situ photothermal nanoreactor with shape selective catalysis for C-C coupling reaction

Carbon-carbon (C-C) coupling reactions represent one of the most powerful tools for the synthesis of complex natural products, bioactive molecules developed as drugs and agrochemicals. In this work, a multifunctional nanoreactor for C-C coupling reaction was successfully fabricated via encapsulating the core-shell Cu@Ni nanocubes into ZIF-8 (Cu@Ni@ZIF-8). In this nanoreactor, Ni shell of the core-shell Cu@Ni nanocubes was the catalytical active center, and Cu core was in situ heating source for the catalyst by absorbing the visible light. Moreover, benefiting from the plasmonic resonance effect between Cu@Ni nanocubes encapsulated in ZIF-8, the absorption range of nanoreactor was widened and the utilization rate of visible light was enhanced. Most importantly, the microporous structure of ZIF-8 provided shape-selective of reactant. This composite was used for the highly shape-selective and stable photocatalysed C-C coupling reaction of boric acid under visible light irradiation. After five cycles, the nanoreactor still remained high catalytical activity. This Cu@Ni@ZIF-8 nanoreactor opens a way for photocatalytic C-C coupling reactions with shape-selectivity.

     

Hybrid-triggered fault detection filter design for networked Takagi–Sugeno fuzzy systems subject to persistent heavy noise disturbance

In the network environment, the single time-triggered scheme wastes limited bandwidth resources due to all the sampled data are transmitted to the networks, and the single event-triggered scheme may increase system error because of ignoring factors such as changes in network utilization. To reduce the design conservatism, this paper is concerned with the hybrid-triggered L₁ fault detection filter design for a class of nonlinear networked control systems (NCSs) described by Takagi–Sugeno (T-S) fuzzy model. Taking the effects of time-triggered scheme and event-triggered scheme into consideration simultaneously, we construct a fuzzy fault detection system. New results on stability and L₁ performance are proposed for fuzzy fault detection system by exploiting the Lyapunov–Krasovskii functional and by means of the integral inequality method. Specially, attention is focused on the design of fault detection filter that guarantees a prescribed L₁ noise attenuation level . Finally, two examples are presented to demonstrate the effectiveness of the proposed method.     

Effects of Agaricus bisporus on gel properties of chicken myofibrillar protein

The gel-forming ability of myofibrillar protein (MP) is highly correlated with the characteristics of emulsified meat products. Incorporation of Agaricus bisporus (Ab) powder into MP gels may enhance its gel properties to facilitate the development of a novel and safe meat product. Therefore, this study investigated the effects of Ab powder on gel strength, water holding capacity (WHC), texture, rheological behaviour, LF-NMR spin–spin relaxation (T₂), microstructure and protein secondary structure of the MP gel system. The results indicated that the gel strength, WHC, G' value and G" value were significantly improved when the addition of Ab powder increased from 0% to 6% (P < 0.05). Meanwhile, the T₂ relaxation time was shortened, and free water was transformed into immobilised water. The texture of the gel was improved when 1%–4% Ab powder was added compared to the control. Furthermore, Ab filled in the gel network and promoted the unfolding of MP α-helix and the formation of MP β-sheet during the thermal denaturation of MP, leading to a dense aggregated network structure. The study suggested that Ab could be a promising ingredient in improving chicken MP's gel properties and developing fat-reduced meat products.     

基于热力学的自然风压分析方法

从热力学的角度出发，考虑巷道热力因素对风流的影响，导出自然风压的计算方法。