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Herein, we show two cases of pillar-layered MOFs which are built solely with one kind of three-dimensional (3D) ditopic ligand. The ligand in both structures functions not only as an intralayer linker in the layer but also as a "pillar" between adjacent layers. Such multi-functionality of the linker is accompanied by uncommon asymmetric 10-c metal hexamer or 7-c tetramer nodes, which have never been reported in previous 3D MOF structures. [ABSTRACT FROM AUTHOR]

Coordination engineering strategy for optimizing the catalytic performance of single‐atom catalysts (SACs) has been rapidly developed over the last decade. However, previous reports on copper SACs for nitrate reduction reactions (NO3RR) have mostly focused on symmetric coordination configurations such as Cu‐N4 and Cu‐N3. In addition, the mechanism in terms of the regulation of coordination environment and catalytic properties of SACs has not been well demonstrated. Herein, we disrupted the local symmetric structure of copper atoms by introducing unsaturated heteroatomic coordination of Cu−O and Cu−N to achieve the coordination desymmetrization of Cu‐N1O2 SACs. The Cu‐N1O2 SACs exhibit an efficient nitrate‐to‐ammonia conversion with a high FE of ~96.5 % and a yield rate of 3120 μg NH3 h−1 cm−2 at −0.60 V vs RHE. As indicated by in situ Raman spectra, the catalysts facilitate the accumulation of NO3− and the selective adsorption of *NO2, which were further confirmed by the theoretical study of surface dipole moment and orbital hybridization. Our work illustrated the correlation between the coordination desymmetrization and the catalytic performance of copper SACs for NO3RR. [ABSTRACT FROM AUTHOR]

Electrochemical nitric oxide reduction reaction (eNORR) is regarded a promising strategy for NO removal and NH3 synthesis. However, current electrocatalysts for NORR encounter problems of low activity and selectivity, also facing the challenge of avoiding competitive hydrogen evolution reaction (HER). Herein, we designed and fabricated CuRh metal alloy nanosheets based on a facile solvothermal method for selective NH2OH* adsorption in eNORR. In situ FTIR spectroscopy revealed that the CuRh nanosheets (CuRh NSs) enhanced the adsorption of NH2OH*, thus promoting the generation of NH4+. CuRh NSs exhibited efficient NORR catalysis with a high faradaic efficiency (FE) of 93.1% and an ammonia yield of 436 μmol h−1 cm−2 at −0.6 V vs. RHE. Our work demonstrated that the introduction of Rh could regulate the electronic structure of Cu in CuRh NSs, optimizing its adsorption ability towards NH2OH*, and improving the catalytic selectivity for ammonia synthesis via eNORR. [ABSTRACT FROM AUTHOR]

Background: The exact pathogenic mechanism of the painful diabetic peripheral neuropathy (DPN) is poorly understood. Our study aimed to evaluate the association amongst vitamin D status, inflammatory cytokines, and painful DPN.Methods: A total of 483 patients were divided into three groups, i.e., diabetes without DPN (no-DPN, n = 86), diabetes with painless DPN (painless DPN, n = 176) and diabetes with painful DPN (painful DPN, n = 221) groups. Basic information and laboratory results were collected. The concentrations of vitamin D (25-hydroxyvitamin D), high-sensitivity C-reactive protein, interleukin (IL)-2, IL-4, IL-6, IL-10, tumor necrosis factor-α (TNF-α), and interferon-γ (IFN-γ) were also measured.Results: The prevalence of severe vitamin D deficiency (