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Electrochemical conversion of nitrate (NO3-) into ammonia (NH3) recycles nitrogen and offers a route to the production of NH3, which is more valuable than dinitrogen gas. However, today's development of NO3- electroreduction remains hindered by the lack of a mechanistic picture of how catalyst structure may be tuned to enhance catalytic activity. Here we demonstrate enhanced NO3- reduction reaction (NO3-RR) performance on Cu50Ni50 alloy catalysts, including a 0.12 V upshift in the half-wave potential and a 6-fold increase in activity compared to those obtained with pure Cu at 0 V vs reversible hydrogen electrode (RHE). Ni alloying enables tuning of the Cu d-band center and modulates the adsorption energies of intermediates such as *NO3-, *NO2, and *NH2. Using density functional theory calculations, we identify a NO3-RR-to-NH3 pathway and offer an adsorption energy-activity relationship for the CuNi alloy system. This correlation between catalyst electronic structure and NO3-RR activity offers a design platform for further development of NO3-RR catalysts.The disproportionation reaction of oxoiron(IV) porphyrin complex (II) to oxoiron(IV) porphyrin π-cation radical complex (I) and iron(III) porphyrin complex (III) have been proposed in various reactions. However, there have been no report that clarifies the disproportionation reaction spectroscopically. Here, we show direct evidence for the disproportionation reaction of II with absorption, 2H NMR, and EPR spectroscopy. Kinetic study of the disproportionation reaction with stopped flow technique can be analyzed as the second-order reaction for the concentration of proton and the first-order for the concentration of II. These results allow us to propose the mechanism of the disproportionation reaction, involving the sequential addition of two protons to the oxo ligand of II, to give an iron(III) porphyrin π-cation radical species, which reacts with another II to afford I and III.The discovery of low-cost, less toxic, and earth-abundant thermoelectric materials is a great challenge. Herein, with the aid of a unique and safe boron-chalcogen method, we discover the new tetragonal α-CsCu5Se3, featuring a previously unrecognized structure in the ternary family of Cs/Cu/Se. The structure is constructed by a Chinese-knot-like Cu8Se8 building unit that is further linked into a 3D network. α-CsCu5Se3 exhibits thermal stability that is superior to that of the recently established thermoelectric materials Cu2-xSe and CsAg5Te3 suffering unfavorable phase transitions. Distinct from the liquidlike migration in Cu2-xSe, α-CsCu5Se3 obeys a typical crystalline solid thermal transport behavior dominated by Umklapp scattering. CADD522 In compariosn to the isostructural CsAg5Te3, α-CsCu5Se3 shows a 30% volume decrease that leads to stronger orbital overlapping that markedly decreases the band effective mass (m*). With a smaller m* and a softer Cu-Se bond, α-CsCu5Se3 eventually realizes a 200% increase in the power factor (8.17 μW/(cm K2), the highest among the copper-rich alkali-metal chalcogenides) and a figure of merit (ZT) of 1.03 at 980 K. Further, the doping in α-Cs(Cu0.96Sb0.04)5Se3 boosts the lattice anharmonicity by the lone pairs that, via intensifying the Umklapp scattering and slowing the phonon velocity, ensures a low lattice thermal conductivity (0.40 W/(m K)), and finally leads to a ZTmax value of 1.30 at 980 K. Our discovery represents a step toward low-cost, earth-abundant, and high-performance chalcogenide materials that will shed useful light on future exploration in the related fields.Perovskite light-emitting diode (PeLED) has been vigorously developed in recent years. As it has demonstrated good performance on the rigid substrates, the next important direction of PeLED is its integration with stretchable components to realize stretchable, responsive device. Here, we describe a facile fabrication of stretchable perovskite light-emissive touch-responsive devices (PeLETDs) by utilizing highly transparent and conductive polyurethane/silver nanowires (PU/AgNWs) as the electrode. Meanwhile, a stretchable tricomposite perovskite emissive layer was developed by blending a small amount of poly(ethylene oxide) (PEO) and poly(vinylpyrrolidone) (PVP) with CsPbBr3. Additionally, a thin PVP layer was introduced at the bottom of the emissive layer. CADD522 On one hand, it can further improve the morphology of the emissive layer; on the other hand, it can serve as an electron-injection barrier to reduce the high nonradiative recombination at the corresponding interface. Further, to fulfill the responsive function of the fabricated PeLEDs, a poly(ethylene terephthalate) (PET) spacer with a 100 μm thickness was inserted between the top electrode and the emissive layer. A stretchable PeLETD is finally demonstrated to possess a low turn-on voltage of 2 V with a brightness of 380.5 cd m-2 at 7.5 V and can sustain 30% uniaxial strain with a small luminance variation of 24%. More interestingly, our stretchable PeLETD exhibited high stability, which could be well touch responsivity, where the luminance is on/off switched for 300 cycles by repeatedly applying pressure.A novel fluorinated biphenyldicarboxylate ligand of 3,3',5,5'-tetrafluorobiphenyl-4,4'-dicarboxylic acid (H2-TFBPDC) and its terbium metal-organic framework, [Tb2(TFBPDC)3(H2O)]·4.5DMF·0.5H2On (denoted as JXNU-6), were synthesized. JXNU-6 exhibits a three-dimensional (3D) framework built from one-dimensional (1D) terbium carboxylate helical chains bridged by TFBPDC2- linkers. The 3D framework of JXNU-6 features 1D fluorine-lined channels. The gas adsorption experiments show that the activated JXNU-6 (JXNU-6a) displays distinct adsorption behavior for propyne (C3H4) and propylene (C3H6) gases. The effective removal of a trace amount of C3H4 from C3H6 was achieved by JXNU-6a under ambient conditions, which is demonstrated by the column-breakthrough experiments. The modeling studies show that the preferential binding sites for C3H4 are the exposed F atoms on the pore surface in 1D channels. The strong C-H···F hydrogen bonds between C3H4 molecules and F atoms of TFBPDC2- ligands dominate the host-guest interactions, which mainly account for the excellent C3H4/C3H6 separation performance of JXNU-6a.
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