Electrochemical CO2 reduction is a key technology to recycle CO2 as a renewable resource, but adsorbing CO2 on the catalyst surface is challenging. We explored the effects of reduced graphene oxide (rGO) in Sn/rGO composites and found that the CO2 adsorption ability of Sn/rGO was almost 4-times higher than that of bare Sn catalysts. Density functional theory calculations revealed that the oxidized functional groups of rGO offered adsorption sites for CO2 toward the adjacent Sn surface and that CO2-rich conditions near the surface facilitated the production of formate via COOH* formation while suppressing CO* formation. Scanning electrochemical cell microscopy directly indicated that CO2 reduction was accelerated at the interface, together with the kinetic suppression of undesirable and competitive hydrogen evolution at the interface. Thus, the synergism of Sn/rGO ensures a substantial/rapid supply of CO2 from the functional groups to the Sn surface, thereby enhancing the Faradaic efficiency 1.8-times compared with that obtained with bare Sn catalysts.

Carbon‐based metal‐free catalysts for the hydrogen evolution reaction (HER) are essential for the development of a sustainable hydrogen society. Identification of the active sites in heterogeneous catalysis is key for the rational design of low‐cost and efficient catalysts. Here, by fabricating holey graphene with chemically dopants, the atomic‐level mechanism for accelerating HER by chemical dopants is unveiled, through elemental mapping with atomistic characterizations, scanning electrochemical cell microscopy (SECCM), and density functional theory (DFT) calculations. It is found that the synergetic effects of two important factors—edge structure of graphene and nitrogen/phosphorous codoping—enhance HER activity. SECCM evidences that graphene edges with chemical dopants are electrochemically very active. Indeed, DFT calculation suggests that the pyridinic nitrogen atom could be the catalytically active sites. The HER activity is enhanced due to phosphorus dopants, because phosphorus dopants promote the charge accumulations on the catalytically active nitrogen atoms. These findings pave a path for engineering the edge structure of graphene in graphene‐based catalysts.

A damage‐free dewatering method, without centrifugation, mechanical squeezing, and solar irradiation, is important for separating solids from pure water and can be used for the production of biomass‐derived renewable fine chemicals, fertilizers, and fuels in biotechnological applications. Herein a damage‐free steam generator constructed by a single sheet of nitrogen‐doped nanoporous graphene and nitrogen‐doped porous graphene foam as hierarchical structures is reported. The multifunctional hierarchical graphene steam generator has a high water evaporation rate (1.54 kg m−2 h−1) accompanied by a high energy conversion efficiency (82.2%). Furthermore, it exhibits excellent persistence in dewatering performance over multiple uses, unlike the graphene foam that shows marked reduction in performance after several reuses. Therefore, the multifunctional hierarchical graphene steam generator is a cost‐effective material for accelerating both the harvesting of biomass concentrates and the production of pure water.