Atomic metal species-based catalysts (AMCs) show remarkable possibilities in various catalytic reactions.T he coordination configuration of the metal atoms has been widely recognized as the determining factor to the electronic structure and the catalytic activity.H owever,t he synergistic effect between the adjacent layers of the multilayered AMCs is always neglected. We reported an atomic Co and Pt co-trapped carbon catalyst, whichexhibits aultrahigh activity for HER in the wide range of pH (h 10 = 27 and 50 mV in acidic and alkaline media, respectively) with ultralow metal loadings (1.72 and 0.16 wt %f or Co and Pt, respectively), which is much superior to the commercial Pt/C.T heoretical analysis reveals that the atomic metals on the inner graphitic layers significantly alter the electronic structure of the outmost layer,thus tailoring the HER activity.T his finding arouses ar e-thinking of the intrinsic activity origins of AMCs and suggests anew avenue in the structure design of AMCs.

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Atomic metal species-based catalysts (AMCs) show remarkable possibilities in various catalytic reactions.T he coordination configuration of the metal atoms has been widely recognized as the determining factor to the electronic structure and the catalytic activity.H owever,t he synergistic effect between the adjacent layers of the multilayered AMCs is always neglected. We reported an atomic Co and Pt co-trapped carbon catalyst, whichexhibits aultrahigh activity for HER in the wide range of pH (h 10 = 27 and 50 mV in acidic and alkaline media, respectively) with ultralow metal loadings (1.72 and 0.16 wt %f or Co and Pt, respectively), which is much superior to the commercial Pt/C.T heoretical analysis reveals that the atomic metals on the inner graphitic layers significantly alter the electronic structure of the outmost layer,thus tailoring the HER activity.T his finding arouses ar e-thinking of the intrinsic activity origins of AMCs and suggests anew avenue in the structure design of AMCs.

Developing efficient hydrogen storage materials and the corresponding methods is the key to successfully realizing the “hydrogen economy”. The ideal hydrogen storage materials should be capable of reversibly ab-/desorbing hydrogen under mild temperatures with high hydrogen capacities. To achieve this target, the ideal enthalpy of adsorption is determined to be 15-50 kJ/mol for hydrogen storage. However, the current mainstream methods, including molecular physisorption and atomic chemisorption, possess either too high or too low enthalpy of hydrogen adsorption, which are not suitable for practical application. To this end, hydrogen storage via molecular chemisorption is perceived to regulate the adsorption enthalpy with intermediate binding energy between the molecular physisorption and atomic chemisorption, enabling the revisable hydrogen ad-/desorption possible under ambient temperatures. In this perspective, we will elaborate the molecular chemisorption as a new conceptual paradigm and materials design to advance future solid-state hydrogen storage.