A Supported Pd₂Dual‐Atom Site Catalyst for Efficient Electrochemical CO₂Reduction

Abstract

Dual-atom site catalysts (DACs) have emerged as an ew frontier in heterogeneous catalysis because the synergistic effect between adjacent metal atoms can promote their catalytic activity while maintaining the advantages of singleatom site catalysts (SACs), like 100 %a tomic utilization efficiency and excellent selectivity.H erein, as upported Pd 2 DACw as synthesized and used for electrochemical CO 2 reduction reaction (CO 2 RR) for the first time.The as-obtained Pd 2 DACe xhibited superior CO 2 RR catalytic performance with 98.2 %C Of aradic efficiency at À0.85 Vv s. RHE, far exceeding that of Pd 1 SAC, and coupled with long-term stability.T he density functional theory (DFT) calculations revealed that the intrinsic reason for the superior activity of Pd 2 DACt owardC O 2 RR was the electron transfer between Pd atoms at the dimeric Pd sites.T hus,P d 2 DACp ossessed moderate adsorption strength of CO*, which was beneficial for CO production in CO 2 RR.

Lattice‐Confined Ir Clusters on Pd Nanosheets with Charge Redistribution for the Hydrogen Oxidation Reaction under Alkaline Conditions

“…[ 10,22–28 ] However, Pd is extremely stable in particular under alkaline conditions. [ 29 ] Hence, we hypothesize it might be an effective strategy that designing Ir/Pd‐based hybrid electrocatalysts with an optimal balance between the adsorption of H ad and OH ad at the heterointerfaces, thereby enhancing the HOR kinetics accordingly. [ 20,22,30–33 ] In addition, engineering epitaxial nanostructures through depositing one nanocrystal on the surface of the other one has been considered as a promising method to develop advanced heterostructured catalysts with superior catalytic performance, [ 34–36 ] in great part due to their well‐defined structures and heterointerfaces.…”

Emerging Dual‐Atomic‐Site Catalysts for Efficient Energy Catalysis

“…Several Fe, Ag, Pd or other metal precursors with dual-atomic structures have been employed. [49,[73][74][75][76] The "precursor-preselected" wet-chemistry strategy was put forward for the first time by Tian et al [49] They chose dicarbonylcyclopentadienyliron (Fe 2 O 4 C 14 H 10 ), in which two Fe atoms were connected by carbonyl, as metal source. The homonuclear metal precursor was mixed with mesoporous carbon nitride (mpg-C 3 N 4 ), followed by pyrolysis under 5% H 2 /Ar at 300 °C to prepare Fe 2 /mpg-C 3 N 4 catalysts.…”

“…Several Fe, Ag, Pd or other metal precursors with dual‐atomic structures have been employed. [ 49,73–76 ] The “precursor‐preselected” wet‐chemistry strategy was put forward for the first time by Tian et al. [ 49 ] They chose dicarbonylcyclopentadienyliron (Fe 2 O 4 C 14 H 10 ), in which two Fe atoms were connected by carbonyl, as metal source.…”

“…In addition, the Pd DASC can also achieve superior performance toward electrocatalytic CO 2 RR with a high CO Faradaic efficiency of 98.2% at −0.85 V (vs. RHE) and excellent long‐term stability. [ 76 ] Such attractive CO 2 RR activity is attributed to the moderate adsorption strength of CO*, induced by the electron transfer between Pd atoms at the Pd 2 sites. Therefore, the adsorption behaviors of CO 2 or intermediates can be tailored by synergetic effect or interaction of dual‐atomic active sites on homonuclear DASCs, achieving high activity and selectivity for CO 2 reduction.…”

Surface Oxidized Ag Nanofilms Towards Highly Effective CO2 Reduction

“…Among the reduction products, such as CO, HCOOH, CH 4 , CH 3 OH, C 2 H 4 and C 2 H 5 OH, [7–11] CO has received great attention because of its high selectivity and great potential for producing high‐value chemicals and hydrocarbon fuels [12–14] . As compared with the other metal or non‐metal catalysts, [15] noble metal catalysts, such as Au, Ag and Pd, have been reported to be more effective to convert CO 2 into CO, [16–21] Especially, Ag has received particular attention due to its excellent performance for CO 2 reduction to CO as well as moderate price [22–25] …”