Exploring N-Containing Compound Catalyst for H 2 S Selective Oxidation: Case Study of TaON and Ta 3 N 5
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Exploring N‑Containing Compound Catalyst for H2S Selective Oxidation: Case Study of TaON and Ta3N5 Huiting Huang1 · Lijuan Shen2 · Shuai Yang1 · Wenjian Hu1 · Lili Zhang3 · Jianyong Feng1 · Lilong Jiang2 · Tao Yu1,4 · Zhaosheng Li1 · Zhigang Zou1,4 Received: 10 June 2020 / Accepted: 14 October 2020 © Springer Science+Business Media, LLC, part of Springer Nature 2020
Abstract In addition to traditional metal oxides, N-containing compound would become efficient catalyst for H 2S selective oxidation. TaON and T a3N5, taking as examples, with porous structure are able to selectively oxidize H 2S into sulfur. TaON exhibits ca. 2S conversion (~ 100%) 99% H2S conversion and ca. 89% sulfur selectivity at 250 ℃, while Ta3N5 exhibits near complete H and 86% sulfur selectivity at 250 ℃. TaON of lower N content shows higher sulfur selectivity (~ 90–100%) above 130 ℃, compared with that (~ 86–95%) over T a3N5. Whereas, T a3N5 of higher N content demonstrates higher H 2S conversion (~ 30–40%) below 160 ℃, compared with that (~ 6–30%) over TaON. Temperature programmed desorption results show that Ta3N5 owns larger amount of acid sites and weaker basic sites than TaON. Over T a3N5, the reactant molecules could dissociatively adsorb on acid sites more frequently and could be easier to move across the weaker basic sites, thus increasing probability for reaction at low temperature. Manipulating both cations and anions in N-containing compound can alter surface property for optimization of selective H2S oxidation. Graphic Abstract
H2S Conversion
40 %
Ta3N5
20 %
TaON 0%
100 oC
120 oC
140 oC
160 oC
Keywords H2S selective oxidation · (Oxy)nitride catalyst · Surface property · TaON · Ta3N5 Electronic supplementary material The online version of this article (https://doi.org/10.1007/s10562-020-03430-6) contains supplementary material, which is available to authorized users. Extended author information available on the last page of the article
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1 Introduction Currently, the majority of global energy supply relies on fossil fuels [1]. As the element sulfur plays a pivotal role in organism, sulfur-containing compounds are subsequently involved in fossil fuels [2]. During the utilization of fossil fuels, sulfur-containing compounds will inevitably release, either corroding the reaction devices and poisoning the catalysts in industrial processes or becoming sulfur oxides after combustion [3]. In the hydrodesulphurization process of fossil fuels, H 2S is a typical component among the produced sulfur-containing compounds, which should be removed before utilization [4, 5]. An efficient desulfurization process is urgent to eliminate H 2S in the released sour gas. Claus process is the mainstream procedure for H 2S removal in chemical industry [6], in which part of the H2S is burned into SO2, H2O and sulfur vapor; then the remaining H 2S reacts with the S O2 over the catalysts to yield more H2O and sulfur vapor. Due to the limit of thermodynamic balance, ~ 2% H 2S will es
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