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The performance of lithium‐metal batteries is severely hampered by uncontrollable dendrite growth and volume expansion on the metal anodes. Inspired by the "blockchain" concept in data mining, here we utilize a conductive polymer‐filled metal–organic framework (MOF) as the lithium host, in which polypyrrole (PPy) serves as the "chain" to interlink Li "blocks" stored in the MOF pores. While the N‐rich PPy guides fast Li+ infiltration/extrusion and serves as the nucleation sites for isotropic Li growth, the MOF pores compartmentalize bulk Li deposition for 3D matrix Li storage, leading to low‐barrier and dendrite‐free Li plating/stripping with superb Coulombic efficiency. The as‐fabricated lithium‐metal anodes operate over 700 cycles at 5 mA cm−2 in symmetric cells, and 800 cycles at 1 C in full cells with a per‐cycle capacity loss of only 0.017 %. This work might open a new chapter for Li‐metal anode construction by introducing the concept of "blockchain" management of Li plating/stripping. [ABSTRACT FROM AUTHOR]

Electrocatalytic conversion of carbon dioxide into high‐value multicarbon (C2+) chemical feedstocks offers a promising avenue to liberate the chemical industry from fossil‐resource dependence and eventually close the anthropogenic carbon cycle but is severely impeded by the lack of high‐performance catalysts. To break the linear scaling relationship of intermediate binding and minimize the kinetic barrier of CO2 reduction reactions, ternary Cu–Au/Ag nanoframes were fabricated to decouple the functions of CO generation and C−C coupling, whereby the former is promoted by the alloyed Ag/Au substrate and the latter is facilitated by the highly strained and positively charged Cu domains. Thus, C2H4 production in an H‐cell and a flow cell occurred with high Faradic efficiencies of 69±5 and 77±2 %, respectively, as well as good electrocatalytic stability and material durability. In situ IR and DFT calculations unveiled two competing pathways for C2H4 generation, of which direct CO dimerization is energetically favored. [ABSTRACT FROM AUTHOR]