A control-theoretic perspective on optimal high-order optimization

Mathematical Programming - We provide a control-theoretic perspective on optimal tensor algorithms for minimizing a convex function in a finite-dimensional Euclidean space. Given a function...     

The Role of Polarization in Photocatalysis

Semiconductor photocatalysis as a desirable technology shows great potential in environmental remediation and renewable energy generation, but its efficiency is severely restricted by the rapid recombination of charge carriers in the bulk phase and on the surface of photocatalysts. Polarization has emerged as one of the most effective strategies for addressing the above‐mentioned issues, thus effectively promoting photocatalysis. This review summarizes the recent advances on improvements of photocatalytic activity by polarization‐promoted bulk and surface charge separation. Highlighted is the recent progress in charge separation advanced by different types of polarization, such as macroscopic polarization, piezoelectric polarization, ferroelectric polarization, and surface polarization, and the related mechanisms. Finally, the strategies and challenges for polarization enhancement to further enhance charge separation and photocatalysis are discussed.     

Synthesis and Applications of SAPO-34 Molecular Sieves

Silicoaluminophosphate zeolite (SAPO-34) has been attracting increasing attention due to its excellent form selection and controllability in the chemical industry, as well as being one of the best industrial catalysts for methanol-to-olefin (MTO) reaction conversion. However, as a microporous molecular sieve, SAPO-34 easily generates carbon deposition and rapidly becomes inactivated. Therefore, it is necessary to reduce the crystal size of the zeolite or to introduce secondary macropores into the zeolite crystal to form a hierarchical structure in order to improve the catalytic effect. In this review, the synthesis methods of conventional SAPO-34 molecular sieves, hierarchical SAPO-34 molecular sieves and nanosized SAPO-34 molecular sieves are introduced, and the properties of the synthesized SAPO-34 molecular sieves are described, including the phase, morphology, pore structure, acid source, and catalytic performance, in particular with respect to the synthesis of hierarchical SAPO-34 molecular sieves. We hope that the review can provide guidance to the preparation of the SAPO-34 catalysts, and stimulate the future development of high-performance hierarchical SAPO-34 catalysts to meet the growing demands of the material and chemical industries.     

Ultrafine PtRu Dilute Alloy Nanodendrites for Enhanced Electrocatalytic Methanol Oxidation

Dilute alloy nanostructures have been demonstrated to possess distinct catalytic properties. Noble-metal-induced reduction is one effective synthesis strategy to construct dilute alloys and modify the catalytic performance of the host metal. Herein, we report the synthesis of ultrafine PtRu dilute alloy nanodendrites (PtRu NDs, molar ratio Ru/Pt is 1:199) by the reduction of Ru^III ions induced by Pt metal. For the methanol oxidation reaction, PtRu NDs showed the highest forward peak current density (2.66 mA cm⁻², 1.14 A/mg_Pt) and the best stability compared to those of pure-Pt nanodendrites (pure-Pt NDs), commercial PtRu/C and commercial Pt/C catalysts.     

Suppressing Universal Cathode Crossover in High-Energy Lithium Metal Batteries via a Versatile Interlayer Design**

The universal cathode crossover such as chemical and oxygen has been significantly overlooked in lithium metal batteries using high-energy cathodes which leads to severe capacity degradation and raises serious safety concerns. Herein, a versatile and thin (≈25 μm) interlayer composed of multifunctional active sites was developed to simultaneously regulate the Li deposition process and suppress the cathode crossover. The as-induced dual-gradient solid-electrolyte interphase combined with abundant lithiophilic sites enable stable Li stripping/plating process even under high current density of 10 mA cm⁻². Moreover, X-ray photoelectron spectroscopy and synchrotron X-ray experiments revealed that N-rich framework and CoZn dual active sites can effectively mitigate the undesired cathode crossover, hence significantly minimizing Li corrosion. Therefore, assembled lithium metal cells using various high-energy cathode materials including LiNi_0.7Mn_0.2Co_0.1O₂, Li_1.2Co_0.1Mn_0.55Ni_0.15O₂, and sulfur demonstrate significantly improved cycling stability with high cathode loading.     

Visible‐Light‐Promoted Iminyl‐Radical Formation from Acyl Oximes: A Unified Approach to Pyridines,Quinolines, and Phenanthridines

A unified strategy involving visible‐light‐induced iminyl‐radical formation has been established for the construction of pyridines, quinolines, and phenanthridines from acyl oximes. With fac‐[Ir(ppy)₃] as a photoredox catalyst, the acyl oximes were converted by 1 e^? reduction into iminyl radical intermediates, which then underwent intramolecular homolytic aromatic substitution (HAS) to give the N‐containing arenes. These reactions proceeded with a broad range of substrates at room temperature in high yield. This strategy of visible‐light‐induced iminyl‐radical formation was successfully applied to a five‐step concise synthesis of benzo[c]phenanthridine alkaloids.     

An Extragradient-Based Alternating Direction Method for Convex Minimization

In this paper, we consider the problem of minimizing the sum of two convex functions subject to linear linking constraints. The classical alternating direction type methods usually assume that the two convex functions have relatively easy proximal mappings. However, many problems arising from statistics, image processing and other fields have the structure that while one of the two functions has an easy proximal mapping, the other function is smoothly convex but does not have an easy proximal mapping. Therefore, the classical alternating direction methods cannot be applied. To deal with the difficulty, we propose in this paper an alternating direction method based on extragradients. Under the assumption that the smooth function has a Lipschitz continuous gradient, we prove that the proposed method returns an \(\epsilon \)-optimal solution within \(O(1/\epsilon )\) iterations. We apply the proposed method to solve a new statistical model called fused logistic regression. Our numerical experiments show that the proposed method performs very well when solving the test problems. We also test the performance of the proposed method through solving the lasso problem arising from statistics and compare the result with several existing efficient solvers for this problem; the results are very encouraging.     

石墨毡载纳米δ-MnO2高性能除铵净水材料研究

首先制备了α-MnO₂纳米花簇、β-MnO₂纳米针和δ-MnO₂微米颗粒三种不同晶型的MnO₂粉末材料，对其结构、形貌及吸附除铵能力进行了表征和测试.结果表明，层间距（7.2Å）大于NH₄⁺直径（2.96Å）和水合NH₄⁺直径（6.62Å）的δ-MnO₂相比其他两种晶型的MnO₂有更高的NH₄⁺吸附量；接着研究采用KMnO₄原位氧化还原法在石墨毡（GF）上直接生长超薄δ-MnO₂纳米片（MnO₂NPs）阵列构筑了石墨毡载纳米MnO₂（MnO₂NPs/GF）多级结构材料，制备简单，无须成型造粒就可直接用作除铵净水材料，研究结果表明，MnO₂NPs/GF不仅具有较高的吸附量（15 mg·g^－1）与良好的选择性，同时还展现了优异的快速吸附和稳定的循环使用性能.MnO₂NPs/GF对水中NH₄⁺的吸附符合准二级动力学模型，其吸附等温线符合Langmuir吸附等温式，是吸附-离子交换法除铵的理想材料.     

Controllable immobilization of polyacrylamide onto glass slide: synthesis and characterization

A novel route was introduced to synthesize dense polyacrylamide (PAM) onto the glass slide surface. To investigate the surface chemistry of the PAM on the glass slides, X-ray photoelectron spectroscopy (XPS) was utilized to obtain detailed chemical state information on the PAM layer constituents. The XPS peak data were consistent with the presented model of the PAM on the glass slide surface. Scanning electron microscopy and atomic force microscope data indicated the presence of PAM on the glass slides, which consist of nodules. The results showed that PAM was successfully immobilized onto glass slides with a two-tier structure under aqueous condition and a monolayer structure under anhydrous condition. Compared with those under aqueous condition, the controllability of the molecular layer on glass slides and the reproducibility under anhydrous condition were much better, which makes anhydrous condition an advisable condition for the study of the reaction mechanisms of glass slides modified by PAM.     

Rapid detection of pesticide residues in Chinese herbal medicines by molecularly imprinted membrane electrospray ionization mass spectrometry

Chinese herbal medicines(CHMs) play an increasingly important role in the field of medicine and affects public health in the world.Although more and more strict has been employed to ensure the quality and safety of CHMs,pesticide residues in CHMs remain a serious issue and are the bottleneck for the global development of CHMs.In this work,we applied molecularly imprinted membrane electrospray mass spectrometry(MIM-ESI MS) for rapid detecting 4 classes of pesticide residues in CHMs,including organophosphorus(OPP),carbamates,pyrethroids and neonicotinoids in CHMs.Compared with our previous ambient ionization method MESI,MIM-ESI is capable of achieving a ～50-fold increase in the detection limit of conventional analytical methods owing to the specificity recognition and unique enrichment of MIM.The optimal experimental conditions were determined,and the method was further validated for its sensitivity and specificity.Our data showed that MIM-ESI MS is applicable for the direct quantitation of pesticide residues in CHMs.This detection technology may help to ensure the quality of CHMs in the future.