Electrochemical reduction of carbon dioxide (CO2) to fuels and value‐added industrial chemicals is a promising strategy for keeping a healthy balance between energy supply and net carbon emissions. Here, the facile transformation of residual Ni particle catalysts in carbon nanotubes into thermally stable single Ni atoms with a possible NiN3 moiety is reported, surrounded with a porous N‐doped carbon sheath through a one‐step nanoconfined pyrolysis strategy. These structural changes are confirmed by X‐ray absorption fine structure analysis and density functional theory (DFT) calculations. The dispersed Ni single atoms facilitate highly efficient electrocatalytic CO2 reduction at low overpotentials to yield CO, providing a CO faradaic efficiency exceeding 90%, turnover frequency approaching 12 000 h?1, and metal mass activity reaching about 10 600 mA mg?1, outperforming current state‐of‐the‐art single atom catalysts for CO2 reduction to CO. DFT calculations suggest that the Ni@N3 (pyrrolic) site favors *COOH formation with lower free energy than Ni@N4, in addition to exothermic CO desorption, hence enhancing electrocatalytic CO2 conversion. This finding provides a simple, scalable, and promising route for the preparation of low‐cost, abundant, and highly active single atom catalysts, benefiting future practical CO2 electrolysis. 相似文献
We present a THz emission enhancement of 41 times at 0.92 THz from a metasurface made of T-shaped resonators excited in a quasi-near-field zone. Such a metasurface has an intrinsic transmission minimum with Q factor of 4 at 1.25 THz under far-field excitation. When this metasurface is coupled onto the backside of a 625-μm-thick photoconductive emitter, the metasurface is below the Fraunhofer distance to the excitation source. As such, one broad enhancement around 0.47 THz and another extremely narrow enhancement at 0.92 THz in the emission spectrum are observed owing to a quasi-near-field excitation. Theoretically, the Q factor of the latter is up to 307, which is limited by the spectral resolution in experiment. The numerical simulations indicate that the T-shaped resonators serve as an array of plasmonic antennas resulting in the aforementioned emission enhancement of THz radiation.