用于从碱性海水中高效电催化析氢的普鲁士蓝类似物的异质结构核壳 Ni-Co@Fe-Co 纳米盒,ACS Catalysis

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用于从碱性海水中高效电催化析氢的普鲁士蓝类似物的异质结构核壳 Ni-Co@Fe-Co 纳米盒
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-01-09 , DOI: 10.1021/acscatal.2c05433
Hao Zhang ₁ , Jiefeng Diao ₂ , Mengzheng Ouyang ₃ , Hossein Yadegari ₁ , Mingxuan Mao ₄ , Mengnan Wang ₁ , Graeme Henkelman ₂ , Fang Xie ₁ , D Jason Riley ₁

Affiliation

合理构建用于析氢反应 (HER) 的高效低成本电催化剂对于海水电解至关重要。在此，使用迭代共沉淀策略合成了基于普鲁士蓝类似物（Ni-Co@Fe-Co PBA）的三金属异质结构核壳纳米盒。相同的共沉淀程序用于制备 PBA 核和壳，壳的合成涉及在引入亚铁离子期间的化学蚀刻。由于其独特的结构和组成，优化后的三金属Ni-Co@Fe-Co PBA具有更多的活性界面位点和高比表面积。因此，^–2分别在碱性淡水和模拟海水中。Operando 拉曼光谱证明了在 HER 过程中催化剂中Co ²⁺从 Co ^{3+的演变。}密度泛函理论模拟表明，H*-N 吸附位点降低了限速步骤的势垒能，引入的 Fe 物种提高了 Ni-Co@Fe-Co PBA 的电子迁移率。核-壳界面处的电荷转移导致 H* 中间体的产生，从而增强 HER 活性。通过将这种 HER 催化剂（Ni-Co@Fe-Co PBA）与我们小组报道的另一种核-壳 PBA OER 催化剂（NiCo@A-NiCo-PBA-AA）配对，发现制造的双电极电解槽实现了高输出电流密度为 44 和 30 mA cm ^–2在碱性淡水和模拟海水中分别在 1.6 V 的低电压下，在 100 小时的测试中表现出卓越的耐久性。

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Heterostructured Core–Shell Ni–Co@Fe–Co Nanoboxes of Prussian Blue Analogues for Efficient Electrocatalytic Hydrogen Evolution from Alkaline Seawater

The rational construction of efficient and low-cost electrocatalysts for the hydrogen evolution reaction (HER) is critical to seawater electrolysis. Herein, trimetallic heterostructured core–shell nanoboxes based on Prussian blue analogues (Ni–Co@Fe–Co PBA) were synthesized using an iterative coprecipitation strategy. The same coprecipitation procedure was used for the preparation of the PBA core and shell, with the synthesis of the shell involving chemical etching during the introduction of ferrous ions. Due to its unique structure and composition, the optimized trimetallic Ni–Co@Fe–Co PBA possesses more active interfacial sites and a high specific surface area. As a result, the developed Ni–Co@Fe–Co PBA electrocatalyst exhibits remarkable electrocatalytic HER performance with small overpotentials of 43 and 183 mV to drive a current density of 10 mA cm^–2 in alkaline freshwater and simulated seawater, respectively. Operando Raman spectroscopy demonstrates the evolution of Co²⁺ from Co³⁺ in the catalyst during HER. Density functional theory simulations reveal that the H*–N adsorption sites lower the barrier energy of the rate-limiting step, and the introduced Fe species improve the electron mobility of Ni–Co@Fe–Co PBA. The charge transfer at the core–shell interface leads to the generation of H* intermediates, thereby enhancing the HER activity. By pairing this HER catalyst (Ni–Co@Fe–Co PBA) with another core–shell PBA OER catalyst (NiCo@A-NiCo-PBA-AA) reported by our group, the fabricated two-electrode electrolyzer was found to achieve high output current densities of 44 and 30 mA cm^–2 at a low voltage of 1.6 V in alkaline freshwater and simulated seawater, respectively, exhibiting remarkable durability over a 100 h test.

更新日期：2023-01-09

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