A Highly Efficient Pt/TiO2-NaY-x Catalyst for RWGS reaction: Enhancement Effect of Adsorbent NaY-x on CO2 Hydrogenation Conversion

Qiuming Zhou , Shuaishuai Lyu , Hongwei Li , Congcong Niu , Rongjun Zhang , Chaopeng Hou , Binhang Yan , Sen Wang , Bo Peng , Run Xu , Mingfeng Li
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Abstract

Selective removal of H2O in-situ from the reverse water gas shift (RWGS) reaction system is an effective approach to intensify the CO2 conversion dictated by thermodynamics. Here, a composite material is prepared by combining a water adsorbent zeolite NaY-2 which modified by hydrothermal treatment at 500°C with Pt/TiO2 catalyst. The synthesized Pt/TiO2-NaY-2 exhibits much higher activity and CO selectivity than conventional Pt/TiO2. It shows the highest CO2 conversion of 42.3% and consistently exceeds the corresponding thermodynamic equilibrium conversion (28.6%) over 120 h on stream with 100% CO selectivity at 340°C. The persistent catalytic enhancement is mainly attributed to the well aligning between the desorption temperature of H2O on NaY-2 (270°C, 330°C) and the reaction temperature. The introduced NaY-2 demonstrates an electronic effect on Pt/TiO2 during the reduction process and generates an electron-rich Pt species. The created Ptδ− sites on Pt/TiO2-NaY-2 possess higher intrinsic catalytic activity than Pt0 sites on Pt/TiO2. The interaction also reduces Pt average particle size and thus weakens the adsorption of CO on Pt, which inhibits the methanation side reaction then improves the CO selectivity on Pt/TiO2-NaY-2. The RWGS reactions on the synthesized Pt-based catalysts proceed through intermediate decomposition mechanism exposed by in-situ IR spectroscopy. The findings of this work provide information of high interest to guide future research on RWGS reaction intensified process via in-situ removal of H2O.

Abstract Image

一种用于RWGS反应的高效Pt/TiO2-NaY-x催化剂:吸附剂NaY-x对CO2加氢转化的增强作用
从逆向水煤气变换(RWGS)反应体系中,原位选择性脱除H2O是强化CO2转化的有效途径。本文将500℃水热改性的吸水性沸石NaY-2与Pt/TiO2催化剂结合制备复合材料。合成的Pt/TiO2- nay -2具有比常规Pt/TiO2更高的活性和CO选择性。结果表明,在340℃下,在100% CO选择性的条件下,在120 h内CO2转化率最高达42.3%,并始终超过相应的热力学平衡转化率(28.6%)。持续的催化增强主要是由于H2O在NaY-2上的解吸温度(270℃、330℃)与反应温度之间的良好匹配。引入的NaY-2在还原过程中对Pt/TiO2产生了电子效应,生成了富电子的Pt物质。在Pt/TiO2- nay -2上生成的Ptδ−位点比在Pt/TiO2上生成的Pt0位点具有更高的本征催化活性。这种相互作用还降低了Pt的平均粒径,从而减弱了CO在Pt上的吸附,抑制了甲烷化副反应,提高了CO在Pt/TiO2-NaY-2上的选择性。在合成的pt基催化剂上,RWGS反应通过原位红外光谱揭示的中间分解机理进行。本研究结果对指导RWGS原位脱水强化反应过程的研究具有重要意义。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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