Rational design of non‐noble metal catalysts with robust and durable electrocatalytic activity for oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER) is extremely important for renewable energy conversion and storage, regenerative fuel cells, rechargeable metal–air batteries, water splitting etc. In this work, a unique hybrid material consisting of Fe3C and Co nanoparticles encapsulated in a nanoporous hierarchical structure of N‐doped carbon (Fe3C‐Co/NC) is fabricated for the first time via a facile template‐removal method. Such an ingenious structure shows great features: the marriage of 1D carbon nanotubes and 2D carbon nanosheets, abundant active sites resulting from various active species of Fe3C, Co, and NC, mesoporous carbon structure, and intimate integration among Fe3C, Co, and NC. As a multifunctional electrocatalyst, the Fe3C‐Co/NC hybrid exhibits excellent performance for ORR, OER, and HER, outperforming most of reported triple functional electrocatalysts. This study provides a new perspective to construct multifunctional catalysts with well‐designed structure and superior performance for clean energy conversion technologies.

Efficient electron transfer for high photocatalytic H2 evolution was obtained by immobilizing ZnS nanoparticles on the nanosheets of graphene and MoS2.

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Unraveling structure-related reconstruction during oxygen evolution reaction (OER) and its correlation with intrinsic electrocatalytic activity is of great significance for designing better catalysts but unfortunately remains elusive. Herein, ultrathin Ni-Fe layered-double-hydroxides (LDH) with inherent oxygen vacancies (V O ) are successfully fabricated via coprecipitation under a controlled manner, which accomplish a quite low overpotential of 230 mV at 10 mA cm −2 in 1.0 M KOH and perform among the best of recently reported nonprecious electrocatalysts. During the OER, inherent V O is experimentally and theoretically evidenced to boost surface reconstruction and the operando formation of p−n interfaces (i.e., γ-Ni-Fe LDH/α-Ni-Fe LDH) via deprotonation. On such reconstructed interfaces, the V O in both surface γ-Ni-Fe LDH and bulk α-Ni-Fe LDH can alter the electron densities of metal sites and subsequently optimize the free energies of a multistep OER pathway, which accounts for the boosted OER activity and, more importantly, identifies the correlation of electrocatalysis with both the catalyst surface and bulk.

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