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Unveiling the role of bisulfide in the photocatalytic splitting of H2S in aqueous solutions
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-03-27 , DOI: 10.1016/j.apcatb.2020.118886
Habeebllah Oladipo , Corrado Garlisi , Jacinto Sa , Erik Lewin , Khalid Al-Ali , Giovanni Palmisano

Anaerobic photocatalytic conversion of aqueous H2S to H2 was tested on Pt-decorated N-doped TiO2 grown on graphene. The hydrogen production increased linearly (rate: 32.3 μmol/h/g, quantum yield: 1.4 × 10–4) with HS concentration, until the critical value of 0.029 mol/dm3, after which it declined to negligible values. The latter was attributed to photon-blockage caused by sulfur-containing species formed on catalyst surface, which could be removed by simple washing of the catalyst leading to its regeneration, as highlighted by the characterization of fresh and used catalyst. Similar tests performed at constant HS concentration and variable pH did not yield a correlation, thus suggesting HS as the major source of H2, and not H+. A new kinetic model assessing the competitive adsorption mechanism reiterated the important role of sulfide ionic species in hydrogen production. A strong correlation between the latter and HS concentration was established based on the reactivity results and proposed mechanism.



中文翻译:

揭示了硫化氢在水溶液中H 2 S光催化裂解中的作用

在生长于石墨烯上的Pt装饰的N掺杂的TiO 2上测试了H 2 S水溶液向H 2的厌氧光催化转化。氢生产线性增加(率:32.3微摩尔/小时/克,量子产率:1.4×10 -4)与HS -浓度,直到0.029摩尔/分米临界值3,在这之后拒绝可以忽略不计的值。后者归因于由在催化剂表面上形成的含硫物质引起的光子阻滞,可以通过简单洗涤催化剂以使其再生来清除光子,正如新鲜和使用过的催化剂的特征所强调的那样。在恒定HS下执行的类似测试-浓度和不同的pH没有产生的相关性,从而表明HS -作为H的主要来源2,和不为H +。评估竞争性吸附机理的新动力学模型重申了硫化物离子物种在制氢中的重要作用。后者和HS之间的强相关性-基于所述反应的结果和提出的机制建立的浓度。

更新日期:2020-03-27
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