通过原子层沉积 MoS2 上的碘化物氧化反应实现高效太阳能燃料生产,Carbon Energy

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通过原子层沉积 MoS2 上的碘化物氧化反应实现高效太阳能燃料生产
Carbon Energy ( IF 19.5 ) Pub Date : 2023-04-04 , DOI: 10.1002/cey2.366
Young Sun Park ₁ , Gyumin Jang ₁ , Inkyu Sohn ₂ , Hyungsoo Lee ₁ , Jeiwan Tan ₁ , Juwon Yun ₁ , Sunihl Ma ₁ , Jeongyoub Lee ₁ , Chan Uk Lee ₁ , Subin Moon ₁ , Hayoung Im ₁ , Seung‐Min Chung ₂ , Seungho Yu ₃ , Hyungjun Kim ₂ , Jooho Moon ₁

Affiliation

析氧反应（OER）作为水分解的半阳极反应，由于其热力学和动力学限制而阻碍了整体反应效率。碘化物氧化反应（IOR）具有低热力学势垒和快速反应动力学，是 OER 的有前途的替代品。在此，我们提出了一种二硫化钼 (MoS ₂ ) 电催化剂，可用于实现 IOR 的高效且非常耐用的阳极。通过原子层沉积在多孔碳纸上沉积的MoS ₂纳米片，由于多孔基材以及固有的碘化物氧化，在阳极电位为 0.63 V 时，相对于可逆氢电极的 IOR 电流密度为 10 mA cm ^–2理论计算证实了MoS _{2的能力。}在 IOR 电催化过程中，对 MoS _{2基异质结构施加较低的正电势，可防止 MoS}₂上活性位点的劣化，从而实现 200 小时的出色耐用性。随后，我们制造了一个双电极系统，包括用于 IOR 的 MoS ₂阳极和用于析氢反应的商业 Pt@C 催化剂阴极。此外，由该电解槽和单个钙钛矿光伏电池组成的光伏电化学制氢装置在无偏条件下在 1 个太阳下显示出 21 mA cm ^{–2的创纪录高电流密度。}

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Efficient solar fuel production enabled by an iodide oxidation reaction on atomic layer deposited MoS2

Oxygen evolution reaction (OER) as a half-anodic reaction of water splitting hinders the overall reaction efficiency owing to its thermodynamic and kinetic limitations. Iodide oxidation reaction (IOR) with low thermodynamic barrier and rapid reaction kinetics is a promising alternative to the OER. Herein, we present a molybdenum disulfide (MoS₂) electrocatalyst for a high-efficiency and remarkably durable anode enabling IOR. MoS₂ nanosheets deposited on a porous carbon paper via atomic layer deposition show an IOR current density of 10 mA cm^–2 at an anodic potential of 0.63 V with respect to the reversible hydrogen electrode owing to the porous substrate as well as the intrinsic iodide oxidation capability of MoS₂ as confirmed by theoretical calculations. The lower positive potential applied to the MoS₂-based heterostructure during IOR electrocatalysis prevents deterioration of the active sites on MoS₂, resulting in exceptional durability of 200 h. Subsequently, we fabricate a two-electrode system comprising a MoS₂ anode for IOR combined with a commercial Pt@C catalyst cathode for hydrogen evolution reaction. Moreover, the photovoltaic–electrochemical hydrogen production device comprising this electrolyzer and a single perovskite photovoltaic cell shows a record-high current density of 21 mA cm^–2 at 1 sun under unbiased conditions.

更新日期：2023-04-04

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