Cr 掺杂剂诱导 Ni2P 纳米晶体的晶体取向和形状调制，用于改善甲醇电合成甲酸盐以及氢气生产,Journal of Materials Chemistry A

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Cr 掺杂剂诱导 Ni2P 纳米晶体的晶体取向和形状调制，用于改善甲醇电合成甲酸盐以及氢气生产
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2024-04-01 , DOI: 10.1039/d4ta01147c
Umesh P. Suryawanshi ₁ , Uma V. Ghorpade ₂ , Jodie A. Yuwono ₃ , Priyank V. Kumar ₂ , Mayur A. Gaikwad ₁ , Seung Wook Shin ₄ , Jun Sung Jang ₁ , Hyo Rim Jung ₁ , Mahesh P. Suryawanshi ₅ , Jin Hyeok Kim ₁

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使用电解技术同时改进电化学甲醇氧化反应（MOR）和析氢反应（HER）是一项重要但具有挑战性的任务。为了解决这个问题，我们报道了 Ni ₂ P 纳米晶体 (NC) 中 Cr 掺杂诱导的晶体取向和形状调制的胶体合成，作为一种先进的双功能电催化剂，用于从阳极的 MOR 和阴极的氢气电合成增值甲酸盐。我们证明，使用 Cr 掺杂 Ni _{2 P 纳米棒（NR）作为双功能催化剂的双电极整体甲醇分解（OMeS）系统可以实现 1.16 V 的最低电压，从而达到 10 mA cm}^-2的电流密度。整个水分解的电池电压为 1.65 V。综合实验和理论研究表明，Cr掺杂剂会诱导Ni ₂ P的形状调制和晶体取向，这有利于MOR中的脱氢过程和HER中的氢吸附的热力学，从而增强电催化活性。有趣的是，使用商用硅光伏电池与采用双功能Cr掺杂Ni ₂ P NR的OMeS电池集成制造的概念验证太阳能驱动系统产生了~12.3 mA cm ^-2的稳定光电流密度60分钟，展示了其在节能和选择性电合成方面的前景，能够以可持续的方式生产有价值的化学品和清洁氢气。

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Cr-dopant induced crystal orientation and shape modulation in Ni2P nanocrystals for improving electrosynthesis of methanol to formate coupled with hydrogen production

Simultaneously improving the electrochemical methanol oxidation reaction (MOR) and hydrogen evolution reaction (HER) using the electrolysis technique is a significant yet challenging task. To tackle this, we report a colloidal synthesis of Cr-dopant induced crystal orientation and shape modulation in Ni₂P nanocrystals (NCs) as an advanced bifunctional electrocatalyst for electrosynthesis of value-added formate from the MOR at the anode and hydrogen at the cathode. We demonstrate that a two-electrode overall methanol splitting (OMeS) system using Cr-doped Ni₂P nanorods (NRs) as a bifunctional catalyst can achieve a lowest voltage of 1.16 V to reach a current density of 10 mA cm⁻², compared to the cell voltage of 1.65 V for overall water splitting. Combined experimental and theoretical investigations revealed that the Cr-dopant induces shape modulation and crystal orientation in Ni₂P, which favors the thermodynamics of the dehydrogenation process in the MOR and hydrogen adsorption in the HER, leading to enhanced electrocatalytic activities. Interestingly, a proof-of-concept solar-driven system fabricated using a commercial Si photovoltaic cell integrated with an OMeS cell employing bifunctional Cr-doped Ni₂P NRs generated a stable photocurrent density of ∼12.3 mA cm⁻² for 60 min., demonstrating its promise for energy-efficient and selective electrosynthesis, enabling the production of valuable chemicals and clean hydrogen in a sustainable manner.

更新日期：2024-04-01

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