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变废为宝:废弃烟头衍生的无金属富氮碳催化剂用于选择性催化氧化硫化氢为硫。

Waste to Wealth: Discarded Cigarette Butt-Derived Metal-Free N-Rich Carbon Catalysts for the Selective Catalytic Oxidation of Hydrogen Sulfide to Sulfur.

机构信息

School of Chemistry and Environment, Yunnan Minzu University, Kunming, Yunnan 650504, PR China.

Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming, Yunnan 650500, PR China.

出版信息

Environ Sci Technol. 2024 Nov 12;58(45):20267-20276. doi: 10.1021/acs.est.4c06461. Epub 2024 Oct 30.

DOI:10.1021/acs.est.4c06461
Abstract

The selective catalytic oxidation of toxic gas HS to elemental sulfur (HS-SCO) is a promising desulfurization process known for its dual benefits of recovering valuable sulfur resources and mitigating environmental pollution. Nevertheless, developing cost-effective and efficient catalysts for HS-SCO remains a significant challenge. In this study, we synthesized a low-cost and metal-free nitrogen-rich carbon catalyst (NrCC) by copyrolyzing discarded cigarette butts (organic solid wastes that are difficult to degrade naturally) with urea for the continuous HS-SCO process at a relatively low temperature. The NrCC exhibited exceptional catalytic performance, achieving complete HS conversion to sulfur at 180 °C, and demonstrated excellent stability in humid (RH = 80%) and high CO concentration environments. The catalyst succeeded due to its developed pore structure (specific surface area as high as 2267.77 m·g) and abundant pyridine-N sites. DFT calculations showed that the pyridine-N neighbor carbon sites were the active sites promoting HS adsorption and dissociation. This study presents a novel "waste control by waste" strategy that integrates the utilization of organic solid waste resources with air pollution control measures, showcasing the potential for sustainable environmental solutions.

摘要

有毒气体 H2S 选择性催化氧化为元素硫(HS-SCO)是一种很有前途的脱硫工艺,具有回收有价值的硫资源和减轻环境污染的双重好处。然而,开发经济高效的 HS-SCO 催化剂仍然是一个重大挑战。在这项研究中,我们通过共热解废弃的烟头(一种难以自然降解的有机固体废物)和尿素,合成了一种低成本、无金属的富氮碳催化剂(NrCC),用于在相对较低的温度下连续进行 HS-SCO 工艺。NrCC 表现出了出色的催化性能,在 180°C 时可将 H2S 完全转化为硫,并在潮湿(RH=80%)和高 CO 浓度环境中表现出优异的稳定性。该催化剂之所以成功,是因为其发达的孔结构(比表面积高达 2267.77 m·g)和丰富的吡啶-N 位。DFT 计算表明,吡啶-N 相邻的碳位是促进 H2S 吸附和离解的活性位。本研究提出了一种新颖的“废物控制废物”策略,将有机固体废物资源的利用与空气污染控制措施相结合,展示了可持续环境解决方案的潜力。

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