Evaluating and clustering retrosynthesis pathways with learned strategy

With recent advances in the computer-aided synthesis planning (CASP) powered by data science and machine learning, modern CASP programs can rapidly identify thousands of potential pathways for a given target molecule. However, the lack of a holistic pathway evaluation mechanism makes it challenging to systematically prioritize strategic pathways except for using some simple heuristics. Herein, we introduce a data-driven approach to evaluate the relative strategic levels of retrosynthesis pathways using a dynamic tree-structured long short-term memory (tree-LSTM) model. We first curated a retrosynthesis pathway database, containing 238k patent-extracted pathways along with ∼55 M artificial pathways generated from an open-source CASP program, ASKCOS. The tree-LSTM model was trained to differentiate patent-extracted and artificial pathways with the same target molecule in order to learn the strategic relationship among single-step reactions within the patent-extracted pathways. The model achieved a top-1 ranking accuracy of 79.1% to recognize patent-extracted pathways. In addition, the trained tree-LSTM model learned to encode pathway-level information into a representative latent vector, which can facilitate clustering similar pathways to help illustrate strategically diverse pathways generated from CASP programs.

Tree-structured long short-term memory neural model learns to understand the retrosynthesis design strategies from patent-extracted retrosynthetic pathway data.     

TiO_2/CuPc/NiFe-LDH photoanode for efficient photoelectrochemical water splitting

Photoelectrochemical(PEC) water splitting is a promising approach for renewable hydrogen production.However,the practical PEC solar-to-fuel conversion efficiency is still low owing to poor light absorption and rapid recombination of charge carriers in photoelectrode.In this work,we report a ternary photoanode with simultaneously enhancement of light absorption and water oxidation efficiency by introducing copper phthalocyanine(CuPc) and nickel iron-laye red double hydroxide(NiFe-LDH) on TiO_2(denoted as TiO_2/CuPc/NiFe-LDH).An experimental study reveals that CuPc loading on TiO_2 bring strong visible light absorption;NiFe-LDH as an oxygen evolution reaction catalyst efficiently accelerates the surface water oxidation reaction.This synergistic effect of CuPc and NiFe-LDH gives enhanced photocurrent density(2.10 mA/cm2 at 0.6 V vs.SCE) and excellent stability in the ternary TiO_2/CuPc/NiFeLDH photoanode.     

Insight into Iron Leaching from an Ascorbate-Oxidase-like Fe−N−C Nanozyme and Oxygen Reduction Selectivity**

Ascorbate (H₂A) is a well-known antioxidant to protect cellular components from free radical damage and has also emerged as a pro-oxidant in cancer therapies. However, such “contradictory” mechanisms underlying H₂A oxidation are not well understood. Herein, we report Fe leaching during catalytic H₂A oxidation using an Fe−N−C nanozyme as a ferritin mimic and its influence on the selectivity of the oxygen reduction reaction (ORR). Owing to the heterogeneity, the Fe-N_x sites in Fe−N−C primarily catalyzed H₂A oxidation and 4 e⁻ ORR via an iron-oxo intermediate. Nonetheless, trace O₂⋅⁻ produced by marginal N−C sites through 2 e⁻ ORR accumulated and attacked Fe-N_x sites, leading to the linear leakage of unstable Fe ions up to 420 ppb when the H₂A concentration increased to 2 mM. As a result, a substantial fraction (ca. 40 %) of the N−C sites on Fe−N−C were activated, and a new 2+2 e⁻ ORR path was finally enabled, along with Fenton-type H₂A oxidation. Consequently, after Fe ions diffused into the bulk solution, the ORR at the N−C sites stopped at H₂O₂ production, which was the origin of the pro-oxidant effect of H₂A.     

Co−Co Dinuclear Active Sites Dispersed on Zirconium-doped Heterostructured Co9S8/Co3O4 for High-current-density and Durable Acidic Oxygen Evolution

Developing cost-effective and sustainable acidic water oxidation catalysts requires significant advances in material design and in-depth mechanism understanding for proton exchange membrane water electrolysis. Herein, we developed a single atom regulatory strategy to construct Co−Co dinuclear active sites (DASs) catalysts that atomically dispersed zirconium doped Co₉S₈/Co₃O₄ heterostructure. The X-ray absorption fine structure elucidated the incorporation of Zr greatly facilitated the generation of Co−Co DASs layer with stretching of cobalt oxygen bond and S−Co−O heterogeneous grain boundaries interfaces, engineering attractive activity of significantly reduced overpotential of 75 mV at 10 mA cm⁻², a breakthrough of 500 mA cm⁻² high current density, and water splitting stability of 500 hours in acid, making it one of the best-performing acid-stable OER non-noble metal materials. The optimized catalyst with interatomic Co−Co distance (ca. 2.80 Å) followed oxo-oxo coupling mechanism that involved obvious oxygen bridges on dinuclear Co sites (1,090 cm⁻¹), confirmed by in situ SR-FTIR, XAFS and theoretical simulations. Furthermore, a major breakthrough of 120,000 mA g⁻¹ high mass current density using the first reported noble metal-free cobalt anode catalyst of Co−Co DASs/ZCC in PEM-WE at 2.14 V was recorded.     

运输类飞机机身大开口结构加强方式理论研究

为了对运输类飞机机身大开口结构进行加强,满足刚度连续变形协调的设计要求,本文对机身大开口结构和完整机身结构的刚度进行了深入研究,首先简化了计算模型,对刚度进行了计算,提出了刚度比的定义,得出刚度比与大开口角度、机身半径、蒙皮厚度以及边梁面积之间的关系表达式,得到运输类飞机机身大开口结构加强的原则和方法,在型号上成功得到了应用,用于指导初期的结构设计.     

An approximation-based approach for fuzzy multi-period production planning problem with credibility objective

This paper develops a fuzzy multi-period production planning and sourcing problem with credibility objective, in which a manufacturer has a number of plants or subcontractors. According to the credibility service levels set by customers in advance, the manufacturer has to satisfy different product demands. In the proposed production problem, production cost, inventory cost and product demands are uncertain and characterized by fuzzy variables. The problem is to determine when and how many products are manufactured so as to maximize the credibility of the fuzzy costs not exceeding a given allowable invested capital, and this credibility can be regarded as the investment risk criteria in fuzzy decision systems. In the case when the fuzzy parameters are mutually independent gamma distributions, we can turn the service level constraints into their equivalent deterministic forms. However, in this situation the exact analytical expression for the credibility objective is unavailable, thus conventional optimization algorithms cannot be used to solve our production planning problems. To overcome this obstacle, we adopt an approximation scheme to compute the credibility objective, and deal with the convergence about the computational method. Furthermore, we develop two heuristic solution methods. The first is a combination of the approximation method and a particle swarm optimization (PSO) algorithm, and the second is a hybrid algorithm by integrating the approximation method, a neural network (NN), and the PSO algorithm. Finally, we consider one 6-product source, 6-period production planning problem, and compare the effectiveness of two algorithms via numerical experiments.     

An improved novel joint channel estimation algorithm for the 112 Gbit/s PDM CO-OFDM system

In this paper, an improved novel joint channel estimation algorithm is proposed for the 112 Gbit/s PDM CO-OFDM system. This method combines the advantages of the intra-symbol frequency domain averaging (ISFA) method and the time domain averaging (TA) method, which can realize more accuracy channel estimation. Simulation results show that this proposal could promise a relatively stable performance even under a rapidly time varying environment. It significantly outperforms the ISFA method by 2.2 dB when the DGD equals 1000 ps, and has the advantages of 0.5 dB over ISFA in considering the laser linewidth and frequency offset.     

一种计算多导体传输线电磁脉冲响应的时域方法

基于波形松弛技术, 提出一种计算外界电磁脉冲激励下理想大地上无损多导体传输线瞬态响应的时域迭代方法。首先利用波形松弛技术对复频域内多导体传输线的电报方程进行解耦, 其中相邻导线的耦合作用等效为线上的分布源, 从而使电报方程转换为一系列关于独立导线的解耦方程组; 然后将复频域内传输线的解耦方程转换到时域, 根据时域方程建立相应的等效电路; 最后利用电路仿真软件PSCAD计算电磁脉冲激励下多导体传输线的瞬态响应。本文时域方法的计算结果与时域有限差分(FDTD) 法计算的结果进行对比, 证实了该时域方法的有效性和准确性, 这为工程和科研人员快速评估、分析电磁脉冲激励下多导体传输线的瞬态响应问题提供了一种可靠方法。     

Data analysis method to achieve sub‐10 pm spatial resolution using extended X‐ray absorption fine‐structure spectroscopy

Obtaining sub‐10 pm spatial resolution by extended X‐ray absorption fine structure (EXAFS) spectroscopy is required in many important fields of research, such as lattice distortion studies in colossal magnetic resistance materials, high‐temperature superconductivity materials etc. However, based on the existing EXAFS data analysis methods, EXAFS has a spatial resolution limit of π/2Δk which is larger than 0.1 Å. In this paper a new data analysis method which can easily achieve sub‐10 pm resolution is introduced. Theoretically, the resolution limit of the method is three times better than that normally available. The method is examined by numerical simulation and experimental data. As a demonstration, the LaFe_1–xCr_xO₃ system (x = 0, 1/3, 2/3) is studied and the structural information of FeO₆ octahedral distortion as a function of Cr doping is resolved directly from EXAFS, where a resolution better than 0.074 Å is achieved.     

Ultra-wideband water-based metamaterial absorber with temperature insensitivity

The natural water has frequency dispersion and its permittivity is also related to temperature, which are important factors to design temperature insensitive absorber at microwave frequency. Here, a water-based metamaterial absorber which is fabricated by 3D-printing is proposed. The absorber can perform stably at different temperatures and it also shows 90% absorption in the frequency range of 7.9–21.7 GHz. The experiment proves that the absorber can work at a wide incident angle and is polarization insensitive. Based on these features, the water-based absorber could be applied to various electromagnetic scenarios such as stealth technology and electromagnetic compatibility in temperature-variable environment.