One-pot regenerative CaSO4/CaS-supported γ-Al2O3 catalytic system for sulfur dioxide reduction to elemental sulfur

IF 6.9 2区材料科学 Q2 CHEMISTRY, PHYSICAL Applied Surface Science Pub Date : 2025-08-30 Epub Date: 2025-04-12 DOI:10.1016/j.apsusc.2025.163223

Manjulla Subramaniam , Abdul Rahman Mohamed , Mélanie Emo , Brigitte Vigolo , Pooya Lahijani , Sin Yuan Lai

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Abstract

A revolutionary approach unveiling a novel, sustainable pathway for reducing sulfur dioxide (SO₂) to stable, elemental sulfur by valorizing waste chicken eggshells into highly effective, regenerative calcium sulfate/calcium sulfide-supported γ-alumina (CaSO₄/CaS-γ-Al₂O₃) catalytic system was presented. In this work, composite catalysts of CaO-supported γ-Al₂O₃ (CaO-γ-Al₂O₃) at various CaO loading percentages (30, 50, 70 and 90 wt%) were prepared via impregnation method. The composites improved chemical and structural properties attributed to strong basicity, thereby increasing SO₂ reduction efficiency. At 800 °C and a gas hourly space velocity of 18 L/h·g, the catalyst with 70 wt% CaO-γ-Al₂O₃ achieved optimum conditions, resulting in a high sulfur yield of 85.60 % and SO₂ conversion of 48.99 % after 16.5 h. The reaction mechanistic pathways, including Langmuir–Hinshelwood (L–H), Eley–Rideal (E–R) and Mars-van Krevelen (MvK), revealed a cyclic calcium-based catalytic system supported γ-Al₂O₃ and elemental sulfur production.

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用于将二氧化硫还原为元素硫的单锅再生 CaSO4/CaS-supported γ-Al2O3 催化系统

提出了一种革命性的方法，通过将废鸡蛋壳转化为高效再生硫酸钙/硫化钙负载的γ-氧化铝（CaSO4/CaS-γ-Al2O3）催化体系，揭示了一种新的、可持续的途径，将二氧化硫（SO2）还原为稳定的单质硫。本文采用浸渍法制备了CaO负载率为30、50、70、90 wt%的CaO-γ-Al2O3复合催化剂（CaO-γ-Al2O3）。复合材料由于具有强碱性而改善了化学和结构性能，从而提高了SO2还原效率。在800 °C和18 L/h·g的气时空速下，CaO-γ-Al2O3质量分数为70 wt%的催化剂达到最佳条件，在16.5 h后，硫收率达到85.60 %，SO2转化率达到48.99 %。Langmuir-Hinshelwood （L-H）、Eley-Rideal （E-R）和Mars-van Krevelen （MvK）三种反应途径揭示了一种支持γ-Al2O3和单质硫生成的循环钙基催化体系。

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来源期刊

Applied Surface Science 工程技术-材料科学：膜

CiteScore

12.50

自引率

7.50%

发文量

3393

审稿时长

67 days

期刊介绍： Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.