High-Efficiency Oxygen Reduction to Hydrogen Peroxide Catalyzed by Nickel Single-Atom Catalysts with Tetradentate N2 O2 Coordination in a Three-Phase Flow Cell.,Angewandte Chemie International Edition

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High-Efficiency Oxygen Reduction to Hydrogen Peroxide Catalyzed by Nickel Single-Atom Catalysts with Tetradentate N2 O2 Coordination in a Three-Phase Flow Cell.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-04-27 , DOI: 10.1002/anie.202004841
Yulin Wang _{1,

2} , Run Shi ₁ , Lu Shang ₁ , Geoffrey I N Waterhouse ₃ , Jiaqi Zhao _{1,

2} , Qinghua Zhang ₄ , Lin Gu _{4,

5} , Tierui Zhang _{1,

2}

Affiliation

Carbon‐supported Ni^II single‐atom catalysts with a tetradentate Ni‐N₂O₂ coordination formed by a Schiff base ligand‐mediated pyrolysis strategy are presented. A Ni^II complex of the Schiff base ligand (R ,R )‐(−)‐N,N′‐bis(3,5‐di‐tert‐butylsalicylidene)‐1,2‐cyclohexanediamine was adsorbed onto a carbon black support, followed by pyrolysis of the modified carbon material at 300 °C in Ar. The Ni‐N₂O₂/C catalyst showed excellent performance for the electrocatalytic reduction of O₂ to H₂O₂ through a two‐electron transfer process in alkaline conditions, with a H₂O₂ selectivity of 96 %. At a current density of 70 mA cm⁻², a H₂O₂ production rate of 5.9 mol g_cat.⁻¹ h⁻¹ was achieved using a three‐phase flow cell, with good catalyst stability maintained over 8 h of testing. The Ni‐N₂O₂/C catalyst could electrocatalytically reduce O₂ in air to H₂O₂ at a high current density, still affording a high H₂O₂ selectivity (>90 %). A precise Ni‐N₂O₂ coordination was key to the performance.

中文翻译：

三相流通池中四齿状N2 O2配位的镍单原子催化剂催化的高效氧还原为过氧化氢。

介绍了由席夫碱配体介导的热解策略形成的具有四齿Ni-N ₂ O ₂配位的碳负载Ni ^II单原子催化剂。席夫碱配体（R，R）-（-）-N，N'-双（3,5-二叔丁基水杨基）-1,2-环己二胺的Ni ^II络合物被吸附到炭黑载体上，然后在300°C下在Ar中热解改性碳材料。在Ni-N ₂ ö ₂ / C催化剂表现出优异的性能的电催化还原的O- ₂至H ₂ ö ₂通过在碱性条件下的双电子转移过程，用含H₂ O _2的选择性为96％。在70 mA cm ^-2的电流密度下，H ₂ O _2的生产率为5.9 mol g _cat。使用三相流通池可实现^-1 h ^-1，并在8小时的测试中保持了良好的催化剂稳定性。Ni-N ₂ O ₂ / C催化剂可以在高电流密度下将空气中的O ₂电催化还原为H ₂ O ₂，仍然具有较高的H ₂ O ₂选择性（> 90％）。精确的Ni‐N ₂ O ₂配合对于性能至关重要。

更新日期：2020-04-27

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