Building Up a Picture of the Electrocatalytic Nitrogen Reduction Activity of Transition Metal Single-Atom Catalysts

Journal of the American Chemical Society, Journal Year: 2019, Volume and Issue: 141(24), P. 9664 - 9672

Published: May 30, 2019

The lack of chemical understanding and efficient catalysts impedes the development electrocatalytic nitrogen reduction reaction (eNRR) for ammonia production. In this work, we employed density functional theory calculations to build up a picture (activity trends, electronic origins, design strategies) single-atom (SACs) supported on nitrogen-doped carbons as eNRR electrocatalysts. To construct such picture, work presents systematic studies activity SACs covering 20 different transition metal (TM) centers coordinated by atoms contained in three types carbon substrates, which gives 60 SACs. Our study shows that intrinsic trends could be established basis adatom adsorption energy (ΔEN*). Furthermore, influence support (ligands) ΔEN* proved related bonding/antibonding orbital population regulating scaling relations intermediates, respectively. Accordingly, two-step strategy is proposed improving eNNR TM-SACs, involves following: (i) selection most promising family (g-C3N4 predicted work) (ii) further improvement best candidate aforementioned via tuning strength key intermediates. Also, stability N-doped supports their selectivity comparison competing hydrogen evolution need taken into consideration screening durable candidates. Finally, an effective designing active, stable, selective based mechanistic insights elaborated guide future studies.

Language: Английский

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From Metal–Organic Frameworks to Single‐Atom Fe Implanted N‐doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media

Angewandte Chemie International Edition, Journal Year: 2018, Volume and Issue: 57(28), P. 8525 - 8529

Published: May 9, 2018

It remains highly desired but a great challenge to achieve atomically dispersed metals in high loadings for efficient catalysis. Now porphyrinic metal-organic frameworks (MOFs) have been synthesized based on novel mixed-ligand strategy afford high-content (1.76 wt %) single-atom (SA) iron-implanted N-doped porous carbon (FeSA -N-C) via pyrolysis. Thanks the Fe sites, hierarchical pores, oriented mesochannels and conductivity, optimized FeSA -N-C exhibits excellent oxygen reduction activity stability, surpassing almost all non-noble-metal catalysts state-of-the-art Pt/C, both alkaline more challenging acidic media. More far-reaching, this MOF-based opens avenue precise fabrication of catalysts.

Language: Английский

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Advanced Electrocatalysts with Single-Metal-Atom Active Sites

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 12217 - 12314

Published: Nov. 2, 2020

Electrocatalysts with single metal atoms as active sites have received increasing attention owing to their high atomic utilization efficiency and exotic catalytic activity selectivity. This review aims provide a comprehensive summary on the recent development of such single-atom electrocatalysts (SAECs) for various energy-conversion reactions. The discussion starts an introduction different types SAECs, followed by overview synthetic methodologies control dispersion atomically resolved characterization using state-of-the-art microscopic spectroscopic techniques. In recognition extensive applications electrocatalytic studies are dissected in terms important electrochemical reactions, including hydrogen evolution reaction (HER), oxygen (OER), reduction (ORR), carbon dioxide (CO2RR), nitrogen (NRR). Examples SAECs deliberated each case performance, structure-property relationships, enhancement mechanisms. A perspective is provided at end section about remaining challenges opportunities targeted reaction.

Language: Английский

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Identification of single-atom active sites in carbon-based cobalt catalysts during electrocatalytic hydrogen evolution

Nature Catalysis, Journal Year: 2018, Volume and Issue: 2(2), P. 134 - 141

Published: Dec. 13, 2018

Language: Английский

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Synergistic effect of well-defined dual sites boosting the oxygen reduction reaction

Energy & Environmental Science, Journal Year: 2018, Volume and Issue: 11(12), P. 3375 - 3379

Published: Jan. 1, 2018

Herein, we construct a novel electrocatalyst with Fe–Co dual sites embedded in N-doped carbon nanotubes ((Fe,Co)/CNT), which exhibits inimitable advantages towards the oxygen reduction reaction.

Language: Английский

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