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Pt-O-Cu anchored on Fe2O3 boosting electrochemical water-gas shift reaction for highly efficient H2 generation
Journal of Catalysis ( IF 6.5 ) Pub Date : 2022-11-28 , DOI: 10.1016/j.jcat.2022.11.033
Shenghong Wang , Changan Zhou , Yongda Cao , Lei Song , Lirong Zheng , Kui Ma , Hairong Yue

Electrochemical water–gas shift (EWGS) reaction is an emerging technology with energy-saving and environmental-friendly advantages to produce high-purity hydrogen form the waste gas containing CO. However, it remains a significant challenge to design superior activity and highly durable EWGS electrocatalysts, particularly with low content of noble metals. Herein, a series of Pt-xCu/Fe2O3 (x = 0, 2, 5) catalysts are synthesized by the complexation precipitation method to construct coupling sites between Pt and CuOx, aiming to optimize the adsorption of CO and the activation of OH. The obtained 2.5Pt-2Cu/Fe2O3 catalyst presents a unique Pt-O-Cu structure, delivering a much lowest onset potential, high specific activity, and excellent mass activity (1.5 A·mgPt-1) at 0.73 V (vs. RHE), which is over 15 and 3 times that of commercial Pt/C (20%) and unmodified Pt/Fe2O3 catalyst, respectively. Meanwhile, the in-situ X-ray absorption results demonstrate that the facilitated interaction among the Pt-O-Cu structure promotes the high durability of the 2.5Pt-2Cu/Fe2O3 catalyst and the operability at high potential. More importantly, the moderate binding of CO and moderate activation of OH* are suggested for boosting the reactivity in the CO electro-oxidation reaction. In particular, the fabricated Pt||2.5Pt-2Cu/Fe2O3, employed in coupling the HER and CO electro-oxide reaction, shows a remarkable hydrogen production of about 98 mmolH2·h−1·mgPt−1 at 0.8 V (vs. RHE). This work also definitely confirms the possibility of the catalyst being applied to produce hydrogen under practical conditions with different concentrations of CO, even being applied in the purification of trace CO in a hydrogen-rich atmosphere.



中文翻译:

固定在 Fe2O3 上的 Pt-O-Cu 促进电化学水煤气变换反应以高效生成 H2

电化学水煤气变换 (EWGS) 反应是一种利用含 CO 废气生产高纯度氢气的新兴技术,具有节能环保的优势。然而,设计高活性和高耐久性的 EWGS 仍然是一项重大挑战电催化剂,特别是贵金属含量低的电催化剂。在此,通过络合沉淀法合成了一系列 Pt-xCu/Fe 2 O 3 (x = 0, 2, 5) 催化剂,在 Pt 和 CuOx 之间构建偶联位点,旨在优化 CO 的吸附和活化哦-。得到的2.5Pt-2Cu/Fe 2 O 3催化剂呈现独特的 Pt-O-Cu 结构,在 0.73 V(相对于RHE)下提供极低的起始电位、高比活性和出色的质量活性(1.5 A·mg Pt -1 ),超过 15 和 3分别是商业 Pt/C (20%) 和未改性 Pt/Fe 2 O 3催化剂的倍数。同时,原位X射线吸收结果表明,Pt-O-Cu结构之间促进的相互作用促进了2.5Pt-2Cu/Fe 2 O 3的高耐久性催化剂和高潜力的可操作性。更重要的是,建议适度结合 CO 和适度激活 OH* 以提高 CO 电氧化反应的反应性。特别地,用于耦合 HER 和 CO 电氧化反应的制造的 Pt​​||2.5Pt-2Cu/Fe 2 O 3显示出约 98 mmol H2 ·h -1 ·mg Pt -1在0.8 V(相对于RHE)。这项工作也明确证实了该催化剂在不同浓度CO的实际条件下用于制氢的可能性,甚至可用于富氢气氛中痕量CO的纯化。

更新日期:2022-11-28
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