Atomically Dispersed Ru Species Induced by Strong Metal-Support Interaction for Electrochemical Methane Reforming.

During the high-temperature oxygen evolution reaction for CO electrolysis in solid oxide electrolysis cells (SOECs), the key elementary process of O transfer is restricted by the high anodic oxygen pressure thermodynamically, thus requiring a high external voltage [open-circuit voltage (OCV)] to drive the electrolysis reaction. Herein, electrochemical CH reforming is introduced to the SOEC anode, which remarkably lowers the anodic oxygen pressure and OCV, finally reducing the energy demand from 3.12 to 0.

Constructing Gradient Orbital Coupling to Induce Reactive Metal-Support Interaction in Pt-Carbide Electrocatalysts for Efficient Methanol Oxidation.

Reactive metal-support interaction (RMSI) is an emerging way to regulate the catalytic performance for supported metal catalysts. However, the induction of RMSI by the thermal reduction is often accompanied by the encapsulation effect on metals, which limits the mechanism research and applications of RMSI. In this work, a gradient orbital coupling construction strategy was successfully developed to induce RMSI in Pt-carbide system without a reductant, leading to the formation of L1-PtM-MC (M = Ti, Zr, Hf, V, Nb, Ta, Cr, Mo, and W) intermetallic electrocatalysts.

Metal bond strength regulation enables large-scale synthesis of intermetallic nanocrystals for practical fuel cells.

Structurally ordered L1-PtM (M = Fe, Co, Ni and so on) intermetallic nanocrystals, benefiting from the chemically ordered structure and higher stability, are one of the best electrocatalysts used for fuel cells. However, their practical development is greatly plagued by the challenge that the high-temperature (>600 °C) annealing treatment necessary for realizing the ordered structure usually leads to severe particle sintering, morphology change and low ordering degree, which makes it very difficult for the gram-scale preparation of desirable PtM intermetallic nanocrystals with high Pt content for practical fuel cell applications. Here we report a new concept involving the low-melting-point-metal (M' = Sn, Ga, In)-induced bond strength weakening strategy to reduce E and promote the ordering process of PtM (M = Ni, Co, Fe, Cu and Zn) alloy catalysts for a higher ordering degree.

In Situ Self-Assembled Active and Stable Ir@MnO/LaSrCrIrO Interfaces for CO Electrolysis.

Solid oxide electrolysis cells are prospective approaches for CO utilization but face significant challenges due to the sluggish reaction kinetics and poor stability of the fuel electrodes. Herein, we strategically addressed the long-standing trade-off phenomenon between enhanced exsolution and improved structural stability via topotactic ion exchange. The surface dynamic reconstruction of the MnO/LaSrCrIrO (LSCIr) catalyst was visualized at the atomic scale.

electrochemical reconstruction of SrFeIrMoO perovskite cathode for CO electrolysis in solid oxide electrolysis cells.

Solid oxide electrolysis cells provide a practical solution for the direct conversion of CO to other chemicals (i.e. CO), however, an in-depth mechanistic understanding of the dynamic reconstruction of active sites for perovskite cathodes during CO electrolysis remains a great challenge.

Redox-manipulated RhO nanoclusters uniformly anchored on SrFeRhMoO perovskite for CO electrolysis.

The sluggish reaction kinetics of CO electroreduction in perovskite-based cathodes severely limits the efficiency of solid oxide electrolysis cells (SOECs). The construction of the high-density active sites on the perovskite surface is crucial for promoting CO electrolysis in SOEC. In this study, we explore a redox-induced redispersion strategy to produce RhO nanoclusters uniformly anchored on a SrFeRhMoO (SFRhM) perovskite surface with a high density of 36,000 µm.

A Reconstructed Cu P O Catalyst for Selective CO Electroreduction to Multicarbon Products.

The electrochemical CO reduction reaction (CO RR) over Cu-based catalysts shows great potential for converting CO into multicarbon (C ) fuels and chemicals. Herein, we introduce an A M O structure into a Cu-based catalyst through a solid-state reaction synthesis method. The Cu P O catalyst is electrochemically reduced to metallic Cu with a significant structure evolution from grain aggregates to highly porous structure under CO RR conditions.

Promoting exsolution of RuFe alloy nanoparticles on SrFeRuMoO via repeated redox manipulations for CO electrolysis.

Metal nanoparticles anchored on perovskite through in situ exsolution under reducing atmosphere provide catalytically active metal/oxide interfaces for CO electrolysis in solid oxide electrolysis cell. However, there are critical challenges to obtain abundant metal/oxide interfaces due to the sluggish diffusion process of dopant cations inside the bulk perovskite. Herein, we propose a strategy to promote exsolution of RuFe alloy nanoparticles on SrFeRuMoO perovskite by enriching the active Ru underneath the perovskite surface via repeated redox manipulations.

Platinum-Decorated Ceria Enhances CO Electroreduction in Solid Oxide Electrolysis Cells.

CO electroreduction by solid oxide electrolysis cells (SOECs) can not only attenuate the greenhouse effect, but also convert surplus electrical energy into chemical energy. The adsorption and activation of CO on the cathode play an important role in the SOEC performance. La Sr Co Fe O -Ce Sm O (LSCF-SDC; SDC=samarium-doped ceria) is a promising SOEC cathode.

Atomic-Scale Insight into Exsolution of CoFe Alloy Nanoparticles in La Sr Co Fe Mo O with Efficient CO Electrolysis.

In situ exsolution of metal nanoparticles in perovskite under reducing atmosphere is employed to generate a highly active metal-oxide interface for CO electrolysis in a solid oxide electrolysis cell. Atomic-scale insight is provided into the exsolution of CoFe alloy nanoparticles in La Sr Co Fe Mo O (LSCFM) by in situ scanning transmission electron microscopy (STEM) with energy-dispersive X-ray spectroscopy and DFT calculations. The doped Mo atoms occupy B sites of LSCFM, which increases the segregation energy of Co and Fe ions at B sites and improves the structural stability of LSCFM under a reducing atmosphere.

In Situ Investigation of Reversible Exsolution/Dissolution of CoFe Alloy Nanoparticles in a Co-Doped Sr Fe Mo O Cathode for CO Electrolysis.

Reversible exsolution and dissolution of metal nanoparticles in perovskite has been investigated as an efficient strategy to improve CO electrolysis performance. However, fundamental understanding with regard to the reversible exsolution and dissolution of metal nanoparticles in perovskite is still scarce. Herein, in situ exsolution and dissolution of CoFe alloy nanoparticles in Co-doped Sr Fe Mo O (SFMC) revealed by in situ X-ray diffraction, scanning transmission electron microscopy, environmental scanning electron microscopy, and density functional theory calculations are reported.

Interfacial Enhancement by γ-Al O of Electrochemical Oxidative Dehydrogenation of Ethane to Ethylene in Solid Oxide Electrolysis Cells.

Oxidative dehydrogenation of ethane (ODE) is limited by the facile deep oxidation and potential safety hazards. Now, electrochemical ODE reaction is incorporated into the anode of a solid oxide electrolysis cell, utilizing the oxygen species generated at anode to catalytically convert ethane. By infiltrating γ-Al O onto the surface of La Sr Co Fe O -Sm Ce O (LSCF-SDC) anode, the ethylene selectivity reaches as high as 92.