Anthony Vasileff

Monitoring and controlling the reconstruction of materials under working conditions is crucial for the precise identification of active sites, elucidation of reaction mechanisms, and rational design of advanced catalysts. Herein, a Bi‐based metal–organic framework (Bi‐MOF) for electrochemical CO₂ reduction is selected as a case study. In situ Raman spectra combined with ex situ electron microscopy reveal that the intricate reconstruction of the Bi‐MOF can be controlled using two steps: 1) electrolyte‐mediated dissociation and conversion of Bi‐MOF to Bi₂O₂CO₃, and 2) potential‐mediated reduction of Bi₂O₂CO₃ to Bi. The intentionally reconstructed Bi catalyst exhibits excellent activity, selectivity, and durability for formate production, and the unsaturated surface Bi atoms formed during reconstruction become the active sites. This work emphasizes the significant impact of pre‐catalyst reconstruction under working conditions and provides insight into the design of highly active and stable electrocatalysts through the regulation of these processes.

Monitoring and controlling the reconstruction of materials under working conditions is crucial for the precise identification of active sites, elucidation of reaction mechanisms, and rational design of advanced catalysts. Herein, a Bi‐based metal–organic framework (Bi‐MOF) for electrochemical CO₂ reduction is selected as a case study. In situ Raman spectra combined with ex situ electron microscopy reveal that the intricate reconstruction of the Bi‐MOF can be controlled using two steps: 1) electrolyte‐mediated dissociation and conversion of Bi‐MOF to Bi₂O₂CO₃, and 2) potential‐mediated reduction of Bi₂O₂CO₃ to Bi. The intentionally reconstructed Bi catalyst exhibits excellent activity, selectivity, and durability for formate production, and the unsaturated surface Bi atoms formed during reconstruction become the active sites. This work emphasizes the significant impact of pre‐catalyst reconstruction under working conditions and provides insight into the design of highly active and stable electrocatalysts through the regulation of these processes.

The review presents the important role of oxygen-bound intermediates in directing the selectivity of electrochemical CO ₂ reduction by considering available theoretical calculations, electrochemical measurements and operando spectroscopy observations.

High CO selectivity for the CO₂electroreduction reaction was achieved on Ni–Cu bimetallic catalysts. We observed that changing the Cu content in the catalysts causes charge redistribution which results in a negative correlation with CO selectivity.

Dual-shell structured sodium titanate cubes with oxygen vacancies are rationally designed and synthesized. Various state-of-the-art approaches offer understandings of its enhanced ion kinetics as an anode for sodium-ion battery..

Atomically dispersed Fe immobilized within N-doped carbon nanosheets was synthesized. The synergistic effect between the metal atom and its anchoring framework sites has been investigated for efficient CO ₂ reduction.

Simultaneous oxidation state engineering of Co, N and S for cobalt nitride and sulfide electrocatalysts is demonstrated to facilitate intermediate desorption for OER and HER, leading to efficient overall water electrolysis in a neutral buffer electrolyte.

Simple methods for fabricating highly active and stable bifunctional electrocatalysts for water electrolysis are essential for hydrogen production. A nickel nitride/sulfide electrode (NiNS), whereby Ni₃N and Ni₃S₂ species are interfaced, is synthesized via a one-step calcination process of Ni foam with thiourea in a vacuum-sealed ampoule. The resultant NiNS can be employed directly as a bifunctional electrocatalyst for water splitting with excellent activity toward the hydrogen evolution reaction and oxygen evolution reaction. The significant electrocatalytic performance of NiNS is attributed to the interface between Ni₃N and Ni₃S₂, which functions as the electrochemical active sites and is beneficial for dissociative adsorption of water molecules. Current densities of 12.4 mA cm⁻² and 48.3 mA cm⁻² at 1.8 V are achieved for overall water electrolysis under neutral pH conditions and in seawater, respectively, when NiNS is applied as both the anode and cathode. This performance is significantly better than that of the benchmark Ir–C and Pt–C electrode system. Accordingly, interfacial NiNS is a promising bifunctional candidate for realistic large-scale water electrolysis.

Low concentration tin bronze alloys show high selectivity for CO₂ electroreduction to CO, while high concentration tin bronze alloys show high selectivity for formate.

The development of renewable energy technologies is currently of global concern and calls for the exploration of novel functional materials. During the past decade, bioinspired polydopamine (PDA) has drawn tremendous attention in the advanced materials field. In this review, we provide an overall view of emerging PDA-inspired materials for energy conversion and storage applications. The peculiar advantages of PDA in the elaboration of desired functional materials are highlighted. We focus on the fabrication strategies used for PDA-based materials and their cutting-edge applications as electrocatalysts for oxygen-, hydrogen- and CO₂- involving energy conversion reactions and electrode materials for lithium-ion batteries, lithium–sulfur batteries and sodium-ion batteries. The rational tailoring of structures and atomic level molecular design of PDA-based materials for specific functions are particularly demonstrated by a range of examples.