Comprehensive Understandings into Complete Reconstruction of Precatalysts: Synthesis, Applications, and Characterizations

Abstract

Reconstruction induced by external environment (such as applied voltage bias and test electrolytes) changes catalyst component and catalytic behaviors. Investigations of complete reconstruction in energy conversion recently receive intensive attention, which promote the targeted design of top‐performance materials with maximum component utilization and good stability. However, the advantages of complete reconstruction, its design strategies, and extensive applications have not achieved the profound understandings and summaries it deserves. Here, this review systematically summarizes several important advances in complete reconstruction for the first time, which includes 1) fundamental understandings of complete reconstruction, the characteristics and advantages of completely reconstructed catalysts, and their design principles, 2) types of reconstruction‐involved precatalysts for oxygen evolution reaction catalysis in wide pH solution, and origins of limited reconstruction degree as well as design strategies/principles toward complete reconstruction, 3) complete reconstruction for novel material synthesis and other electrocatalysis fields, and 4) advanced in situ/operando or multiangle/level characterization techniques to capture the dynamic reconstruction processes and real catalytic contributors. Finally, the existing major challenges and unexplored/unsolved issues on studying the reconstruction chemistry are summarized, and an outlook for the further development of complete reconstruction is briefly proposed. This review will arouse the attention on complete reconstruction materials and their applications in diverse fields.

Electrochemical Surface Restructuring of Phosphorus-Doped Carbon@MoP Electrocatalysts for Hydrogen Evolution

“…Recent research on the activity of the HER and oxygen evolution reaction (OER) has suggested that the in situ reconstructed surface of catalysts under electrochemical conditions provides intrinsic active sites for high catalytic activities [ 30 ]. For example, Liu et al discovered that phosphides derived from CoFeO@ black phosphorus (BP) formed during HER catalysis [ 31 ].…”

Sequential self-reconstruction of localized Mo species in hierarchical carbon/Co–Mo oxide heterostructures for boosting alkaline hydrogen evolution kinetics and durability

“…Therefore, it is worth mentioning that the as-obtained 3D heterostructure exhibits multi-level porosities and open channels, which are in favor of the effective solution permeability and gas release for electrocatalytic reactions. 21 The as-obtained Co@NCNT sub-arrays can act as a physical buffer to strengthen the robustness of the entire heterostructure, which is beneficial for the subsequent exploration of dissolution and self-reconstruction mechanisms with structural integrity.…”

“…The dynamic equilibria of redeposition, polymerization, and reduction evolution on the surface promote the formation of active species and maximize the component utilization, improving the efficiency of alkaline HER activity with long-term stability. 21…”

Insight into Structural Evolution, Active Sites, and Stability of Heterogeneous Electrocatalysts

“…In contrast, some studies have reported that the reconstruction that occurs on catalytic materials is irreversible. [41] Due to the complexity of electrocatalysis,m any factors are likely to affect the reversibility of structural evolution. Even for the same type of material and the same reaction, the difference in the electrolytes and the catalyst surface will also [37] with permission.C opyright 2020, Nature Publishing Group.…”