Strain-Regulated Pd/Cu Core/Shell Icosahedra for Tunable Syngas Electrosynthesis from CO₂

Abstract

Introducing surface strain into catalysts would optimize the adsorption energy and surface electronic structure, but it is rarely used in the carbon dioxide reduction reaction (CO 2 RR) to regulate syngas. Herein, we have demonstrated a new class of Pd/Cu core/shell icosahedra (ico) with a tensile-strained Cu shell for efficient syngas production with tunable compositions from the CO 2 RR for the first time. By tuning the composition of Pd/Cu from 2.2 to 4.3 and 6.1, the molar ratio of H 2 /CO in syngas on Pd/ Cu core/shell ico could be tuned from 1/1 to 2/1 and 3/1, respectively. The variable selectivity of the CO 2 RR on Pd/Cu core/shell ico originated from the tensile-strained Cu shell, which synergistically optimizes the binding energy of the intermediate and the electronic structure of catalysts. The work reveals how surface strain regulation accelerates electrocatalytic performance at the molecular level, providing new strategies to regulate CO 2 RR performance.

Recent Advances in Defect and Interface Engineering for Electroreduction of CO₂ and N₂

“…Lattice strain effect is mainly related to the tensile or compressive effect of heterogeneous atoms on bulk atoms, which plays an important role in electrocatalytic reactions by modulating the surface electronic structure of the catalysts and the adsorption capacity of the adsorbate [49][50][51][52][53][54][55] . Recently, by constructing the composition-controllable Pd/Cu core/shell icosahedron, our group proposed a continuous strain regulation strategy to optimize the surface electronic structure and adsorption energy for CO2RR 56 . The surface strain intensity of the Pd/Cu icosahedron can be achieved by changing their composition.…”

Cu–Ni alloy decorating N-doped carbon nanosheets toward high-performance electrocatalysis of mildly acidic CO2reduction

“…[9][10][11] Among these possible pro-ducts, CO is a more accessible product (CO 2 + 2H + + 2e − → CO + H 2 O, −0.11 V vs. RHE) than other multi-carbon products in terms of reaction kinetics and is also an important raw material in industrial production. [12][13][14] Thus, elevating the conversion efficiency of CO 2 reduction into CO is crucial to promote the actual applications of CO 2 RR. 15,16 On one hand, designing effective catalysts for CO 2 RR is still at the center of promoting the conversion efficiency of CO 2 RR.…”

Single-atom Cu anchored on Mo2C boosts nitrite electroreduction to ammonia

“…24 Among them, Cu-SACs have been demonstrated to be active and selective towards the N-cycle electrocatalysis reactions where ammonia is the main reductive product. [25][26][27][28][29][30] In addition, transition metal carbides such as Mo 2 C represent appealing SAC platforms because Mo 2 C not only possesses a high conductivity to favor rapid electrocatalytic kinetics, but also exhibits abundant surface-exposed Mo sites which may cooperate with singleatomic metal sites to synergistically promote the catalytic activity. [31][32][33] As illustrated in Fig.…”