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[Display omitted] • A rich-mesoporous biocarbon (CSKN-15) was synthesized and analyzed. • The ultra-high U-selective electrosorption coefficient from the mixed solution. • The diffusion process of U(VI) into the pores is the key in the electrosorption. • Faradaic reactions were first carefully analyzed in the electrosorption of U(VI). • The formation mechanism of uranium peroxide species was revealed. Constructing the excellent rich-mesoporous carbon and exploring its electrosorption process are keys to promote the electrosorption industrialization of uranium. In this work, we develop a rich-mesoporous biocarbon by using alkali-thermal-pyrolysis and ammonia low-temperature plasma, and then systematically investigate its electrosorption kinetics and mechanism of U(VI) considering a series of Faradaic side reactions. After the above treatment, the electrosorption efficiency of U(VI) onto biocarbon improves from 49.75% to 94.45%, and the ultra-high U-selectivity coefficient (S U/M) is higher than 120 from the mixed solution. The kinetic diffusion process of U(VI) into the pores is crucial, even in different water systems. Importantly, Faradaic side reactions are proved to be non-negligible factors in the electrosorption of uranium. Especially, the oxygen reduction at the cathode can convert dissolved oxygen into H 2 O 2 , which oxides the amorphous electro-reduced U(V, IV) to U(VI), and finally forms crystalline uranium peroxide species. To sum up, this work not only offers an excellent uranium-selectivity electroadsorbent, but firstly confirms the influence of Faradaic side reactions that has been ignored in the current electrosorption of uranium. [ABSTRACT FROM AUTHOR]