Plasma-driven redox mechanism in the reverse water–gas shift reaction over Ni–In intermetallic catalysts†

EES catalysis Pub Date : 2025-07-17 DOI:10.1039/D5EY00101C
Dae-Yeong Kim, Zhang Wenjun, Kaiyue Dong, Bang Lu, Duanxing Li, Satoru Takakusagi, Shinya Furukawa and Tomohiro Nozaki
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Abstract

The reverse water–gas shift (RWGS) reaction has been recognized as a promising strategy for CO2 valorization. However, it faces limitations due to low activity and poor CO selectivity at low temperatures. In this study, we report that plasma can effectively promote the low-temperature RWGS reaction over Ni–In intermetallic catalysts. The formation of the Ni–In intermetallic phases completely suppresses CH4 formation and achieves 100% CO selectivity. Through in situ transmission infrared spectroscopy (TIR) and in situ X-ray absorption fine-structure (XAFS) analysis, we monitored the changes occurring on the catalyst surface during the plasma reaction. The interaction between redox-active sites present in the Ni–In intermetallic catalysts and plasma-activated species lowers the activation energy, thereby facilitating the RWGS reaction at low temperatures. This study offers fundamental insights into how plasma-activated species enhance catalysis and the underlying mechanisms of low-temperature activation in plasma catalysis.

Abstract Image

Ni-In金属间催化剂上逆水气转换反应的等离子体驱动氧化还原机制
逆向水气转换(RWGS)反应被认为是一种很有前途的二氧化碳增值策略。然而,由于低温下活性低和CO选择性差,它面临着局限性。在本研究中,我们报道了等离子体可以有效地促进Ni-In金属间催化剂上的低温RWGS反应。Ni-In金属间相的形成完全抑制了CH4的形成,实现了100%的CO选择性。通过原位红外光谱(TIR)和原位x射线吸收精细结构(XAFS)分析,监测了等离子体反应过程中催化剂表面发生的变化。Ni-In金属间催化剂中存在的氧化还原活性位点与等离子体活化物质之间的相互作用降低了活化能,从而促进了低温下的RWGS反应。这项研究为等离子体活化物质如何增强催化作用以及等离子体催化低温活化的潜在机制提供了基本的见解。
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