Crystal‐Phase‐Engineered High‐Entropy Alloy Aerogels for Enhanced Ethylamine Electrosynthesis from Acetonitrile DOI

Honggang Huang,

Cun Chen,

Chun‐Chi Chang

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(26)

Published: April 16, 2024

Crystal-phase engineering that promotes the rearrangement of active atoms to form new structural frameworks achieves excellent result in field electrocatalysis and optimizes performance various electrochemical reactions. Herein, for first time, it is found different components metallic aerogels will affect crystal-phase transformation, especially high-entropy alloy (HEAAs), whose transformation during annealing more difficult than medium-entropy (MEAAs), but they still show better performance. Specifically, PdPtCuCoNi HEAAs with parent phase face-centered cubic (FCC) PdCu possess 89.24% selectivity, 746.82 mmol h

Language: Английский

Lattice oxygen-mediated electron tuning promotes electrochemical hydrogenation of acetonitrile on copper catalysts DOI Creative Commons
Cong Wei, Yanyan Fang, Bo Liu

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: June 29, 2023

Copper is well-known to be selective primary amines via electrocatalytic nitriles hydrogenation. However, the correlation between local fine structure and catalytic selectivity still illusive. Herein, we find that residual lattice oxygen in oxide-derived Cu nanowires (OD-Cu NWs) plays vital roles boosting acetonitrile electroreduction efficiency. Especially at high current densities of more than 1.0 A cm-2, OD-Cu NWs exhibit relatively Faradic Meanwhile, a series advanced situ characterizations theoretical calculations uncover residues, form Cu4-O configuration, act as electron acceptors confine free flow on surface, consequently improving kinetics hydrogenation catalysis. This work could provide new opportunities further improve performance beyond, by employing oxygen-mediated tuning engineering.

Language: Английский

Citations

29

Electrosynthesis of ethylene glycol from C1 feedstocks in a flow electrolyzer DOI Creative Commons
Rong Xia, Ruoyu Wang, Bjorn Hasa

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: July 29, 2023

Abstract Ethylene glycol is a widely utilized commodity chemical, the production of which accounts for over 46 million tons CO 2 emission annually. Here we report paired electrocatalytic approach ethylene from methanol. Carbon catalysts are effective in reducing formaldehyde into with 92% Faradaic efficiency, whereas Pt at anode enable through methanol partial oxidation 75% efficiency. With membrane-electrode assembly configuration, show feasibility electrosynthesis single electrolyzer. The electrolyzer operates full cell voltage 3.2 V current density 100 mA cm −2 , 60% reduction energy consumption. Further investigations, using operando flow mass spectroscopy, isotopic labeling, and functional theory (DFT) calculations, indicate that desorption *CH OH intermediate crucial step determining selectively towards

Language: Английский

Citations

24

Microenvironment regulation breaks the Faradaic efficiency-current density trade-off for electrocatalytic deuteration using D2O DOI Creative Commons
Meng He, Rui Li, Chuanqi Cheng

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: June 19, 2024

Abstract The high Faradaic efficiency (FE) of the electrocatalytic deuteration organics with D 2 O at a large current density is significant for deuterated electrosynthesis. However, FE and are two ends seesaw because severe evolution side reaction nearly industrial densities. Herein, we report combined scenario nanotip-enhanced electric field surfactant-modified interface microenvironment to enable arylacetonitrile in an 80% −100 mA cm −2 . increased concentration low activation energy due along tips accelerated transfer suppressed by surfactant-created deuterophobic contribute breaking trade-off between density. Furthermore, application our strategy other reactions improved efficiencies rationalizes design concept.

Language: Английский

Citations

14

Spatial decoupling of bromide-mediated process boosts propylene oxide electrosynthesis DOI Creative Commons

Mingfang Chi,

Jingwen Ke,

Yan Liu

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: April 29, 2024

Abstract The electrochemical synthesis of propylene oxide is far from practical application due to the limited performance (including activity, stability, and selectivity). In this work, we spatially decouple bromide-mediated process avoid direct contact between anode propylene, where bromine generated at then transferred into an independent reactor react with propylene. This strategy effectively prevents side reactions eliminates interference stability caused by massive alkene input vigorously stirred electrolytes. As expected, selectivity for reaches above 99.9% a remarkable Faradaic efficiency 91% 750-h (>30 days). When electrode area scaled up 25 cm 2 , 262 g pure obtained after 50-h continuous electrolysis 6.25 A. These findings demonstrate that bromohydrin route represents viable alternative manufacture epoxides.

Language: Английский

Citations

13

Crystal‐Phase‐Engineered High‐Entropy Alloy Aerogels for Enhanced Ethylamine Electrosynthesis from Acetonitrile DOI

Honggang Huang,

Cun Chen,

Chun‐Chi Chang

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(26)

Published: April 16, 2024

Crystal-phase engineering that promotes the rearrangement of active atoms to form new structural frameworks achieves excellent result in field electrocatalysis and optimizes performance various electrochemical reactions. Herein, for first time, it is found different components metallic aerogels will affect crystal-phase transformation, especially high-entropy alloy (HEAAs), whose transformation during annealing more difficult than medium-entropy (MEAAs), but they still show better performance. Specifically, PdPtCuCoNi HEAAs with parent phase face-centered cubic (FCC) PdCu possess 89.24% selectivity, 746.82 mmol h

Language: Английский

Citations

11