Coupling nonstoichiometric Cu2−xSe with stable Cu2Se berzelianite for efficient synergistic electrocatalytic hydrazine-assisted water splitting,Inorganic Chemistry Frontiers

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Coupling nonstoichiometric Cu2−xSe with stable Cu2Se berzelianite for efficient synergistic electrocatalytic hydrazine-assisted water splitting
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2022-09-27 , DOI: 10.1039/d2qi01699k
Xian-Wei Lv ₁ , Qing-Hui Kong ₁ , Xin-Lian Song ₁ , Yu-Ping Liu ₂ , Zhong-Yong Yuan _{1,

2}

Affiliation

Electrochemical overall water splitting for sustainable hydrogen generation is severely hindered by anode water electrooxidation with sluggish kinetics. Thus, using the thermodynamically favorable hydrazine oxidation reaction (HzOR) to substitute the oxygen evolution reaction (OER) has attracted ever-growing attention. Herein, well-defined copper selenide nanoflakes, in situ grown on copper foam (termed Cu_xSe/CF), were synthesized by a one-step selenization strategy, which are composed of nonstoichiometric Cu_2−xSe with stable Cu₂Se berzelianite that show remarkable bifunctional activities for the hydrogen evolution reaction (HER) and HzOR electrocatalysis. Investigations into the mechanisms uncovered that the high copper deficiencies in the Cu_2−xSe phase make it both an excellent electron donor and acceptor, leading to faster electron transfers across the catalyst (electrode)–electrolyte interface, which greatly boosts the reaction kinetics of HER and HzOR processes. Meanwhile, the Cu₂Se berzelianite phase plays a pivotal role in the long-term electrocatalytic operation for the HER and HzOR. Encouraged by this synergistic advantage, the Cu_xSe/CF catalysts were further employed as good bifunctional catalysts for electrocatalytic hydrazine-assisted overall water splitting with a low cell voltage of 0.49 V at 25 mA cm⁻², as well as having good stability over 20 h, which indicates the broad potential for future industrialization of a sustainable hydrogen-based society.

中文翻译：

将非化学计量的 Cu2−xSe 与稳定的 Cu2Se berzelianite 偶联以实现高效的协同电催化肼辅助水分解

用于可持续制氢的电化学整体水分解受到动力学缓慢的阳极水电氧化的严重阻碍。因此，使用热力学有利的肼氧化反应（HzOR）代替析氧反应（OER）引起了越来越多的关注。在此，通过一步硒化策略合成了在泡沫铜上原位生长的明确定义的硒化铜纳米薄片（称为 Cu _x_{Se/CF），其由非化学计量的 Cu 2− x} Se 和稳定的 Cu _2组成Se berzelianite 对析氢反应 (HER) 和 HzOR 电催化具有显着的双功能活性。对机理的研究发现，Cu _{2− x} Se 相中的高铜缺乏使其既是优秀的电子供体又是受体，从而导致更快的电子在催化剂（电极）-电解质界面上转移，从而大大提高了反应动力学。 HER 和 HzOR 过程。同时，Cu ₂ Se berzelianite 相在 HER 和 HzOR 的长期电催化操作中起着关键作用。在这种协同优势的鼓舞下，Cu _xSe/CF 催化剂被进一步用作电催化肼辅助整体水分解的良好双功能催化剂，在 25 mA cm ^-2下具有 0.49 V 的低电池电压，并且在 20 小时内具有良好的稳定性，这表明了广泛的潜力可持续的氢基社会的未来工业化。

更新日期：2022-09-27

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