Local reaction environment in electrocatalysis

Abstract

This review summarizes and analyses the development of local environment modification in promoting e-refinery. The surface structure, interfacial electric field and ion distribution collectively determine the electrolyte–electrode interface.

Stabilizing the oxidation state of catalysts for effective electrochemical carbon dioxide conversion

“…Based on the Gouy–Chapman–Stern electric double layer model, the microenvironment modulation can be categorized into three scales: catalytic surface, Stern layer, and diffusion layer. 141,142 For catalytic surface microenvironment modulation, theoretical computation revealed that the reductive elimination of bridging O atoms on the surface of SnO 2 was thermodynamically energetic at −0.8 V, whereas the free energy of removing bridging OH groups from the surface surpassed 0 eV at specific steps. 143 The thermodynamic energetic barriers to the reductive elimination of OH groups contributed to the theoretical basis for Sn + retention, and its experimental validation was implemented through synthesizing SnO 2 with enriched surface OH groups (Fig.…”

Enhancing H2O2 Electrosynthesis at Industrial-Relevant Current in Acidic Media on Diatomic Cobalt Sites

“…30 This could be attributed to the large overpotential and high concentration of local H + at the electrochemical interface, which unfortunately led to further reduction of H 2 O 2 to water at the active sites. 31,32 Therefore, there is an urgent need to modulate the electronic structure of the cobalt site to ensure high intrinsic ■ RESULTS AND DISCUSSION Computational Catalyst Screening. We first investigated the activity and selectivity of different catalytic centers toward two-electron ORR using DFT calculations.…”

“…Chen et al showed that pyrrole-type CoN 4 exhibited a relatively high H 2 O 2 yield (2032 mg in 90 h), but the overall H 2 O 2 selectivity is less than 80% . This could be attributed to the large overpotential and high concentration of local H + at the electrochemical interface, which unfortunately led to further reduction of H 2 O 2 to water at the active sites. , Therefore, there is an urgent need to modulate the electronic structure of the cobalt site to ensure high intrinsic activity for H 2 O 2 generation in acid while inhibiting H 2 O 2 further reduction to water under practical operating conditions.…”

One-Step Synthesis of Ultrathin High-Entropy Layered Double Hydroxides for Ampere-Level Water Oxidation

“…However, the sluggish kinetics of the oxygen evolution reaction (OER) at the anode side result in increased energy consumption, posing a significant obstacle to its widespread implementation [2][3][4][5]. Therefore, the search for electrocatalysts with excellent OER performance to meet the needs of the future is one of the fundamental driving forces in the materials science community [6][7][8].…”