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Abstract: The core of energy conversion technologies is developing efficient electrocatalysts for a series of electrochemical reactions proceeded on the electrodes. In the past five years, we developed different carbon-based (e.g. heteroatoms doped graphene and carbon nitride) nanomaterials for efficient electrocatalysis like oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). The nature of these electrochemical processes and reactivity origin of corresponding electrocatalysts were revealed by a combination approach of atomic imaging, spectrum characterization, electrochemical measurements, and DFT computation. We focused on correlating the electrocatalytic activities of these catalysts with their electronic and/or structural properties. As a result, we established ORR and HER activity trends for carbon-based materials by linking their apparent activities (e.g. exchange current density) with their intrinsic adsorption energies and electronic structures. Involving in these works, we proposed a design principle to pioneer the development carbon materials as alternatives to metallic catalysts in the energy conversion field. We will also discuss recent debates about the nature of alkaline HER and its theoretical activity descriptor. Biosketch: Yao Zheng received his B.E. and M.E. degrees from Nanjing University of Technology in 2006 and 2009, and PhD from the University of Queensland (Australia) in 2014. Currently he is a DECRA research fellow in University of Adelaide (Australia) working with Professor Shi Zhang Qiao. His research focuses on developing new electrocatalysts for some key electrocatalysis processes like oxygen reduction, hydrogen evolution, and CO2 reduction reactions especially fundamental studies on the mechanism of alkaline hydrogen evolution reaction and product selectivity on CO2 reduction reaction. He has published 52 papers including Nature Energy, Nature Communication, JACS, and Angew. Chem. etc. with 5500 citations and 13 ESI highly citied papers.