Eco-friendly CaO-based catalysts derived from waste oyster shells for the oxidative coupling of methane

IF 2.7 4区 环境科学与生态学 Q3 ENVIRONMENTAL SCIENCES
JeongHyun Cho, Sangwon Kim, Kyung Tae Park, Chang Houn Rhee, Hai Woong Park, Ji Chul Jung
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Abstract

In this study, we developed an economical and eco-friendly high-performance catalyst for the oxidative coupling of methane from waste oyster shells, which cause environmental pollution. The oyster shells were successfully transformed into CaO-based catalysts by the calcining at different temperatures. During calcination process, foreign elements (Na, Mg, and Al) naturally present in waste oyster shells caused the generation of oxygen vacancies and changes in the surface chemical properties (base sites and surface oxygen species) of the catalysts. When the catalysts were used in oxidative methane coupling, the oxygen vacancies on the catalyst surface played a crucial role in the conversion of methane to methyl radicals, which are expected to dimerize to ethane. However, the moderately basic sites and electrophilic lattice oxygen species facilitated the production of ethylene through the dehydrogenation of ethane. Therefore, the sample calcined at 800 °C not only exhibited an outstanding catalytic activity in the oxidative coupling of methane but also high long-term stability because of its abundant active sites: oxygen vacancies, moderately basic sites, and electrophilic lattice oxygen species. The study demonstrates that waste oyster shells can be successfully recycled into a high value-added product, such as a catalyst applicable in the oxidative coupling of methane.

Graphical abstract

从废牡蛎壳中提取用于甲烷氧化偶联的环保cao基催化剂
在本研究中,我们开发了一种经济环保的高性能催化剂,用于处理废弃牡蛎壳中甲烷的氧化偶联,这对环境造成了污染。通过不同温度下的煅烧,成功地将牡蛎壳转化为cao基催化剂。在煅烧过程中,天然存在于废牡蛎壳中的外来元素(Na、Mg、Al)引起了氧空位的产生,并改变了催化剂的表面化学性质(碱基和表面氧的种类)。当催化剂用于氧化甲烷偶联时,催化剂表面的氧空位对甲烷转化为甲基自由基起着至关重要的作用,甲基自由基有望二聚生成乙烷。中等碱性位和亲电晶格氧有利于乙烷脱氢制乙烯。因此,在800℃下煅烧的样品不仅在甲烷氧化偶联中表现出出色的催化活性,而且由于其丰富的活性位点:氧空位、中等碱性位点和亲电晶格氧种,具有很高的长期稳定性。该研究表明,废弃牡蛎壳可以成功回收为高附加值产品,例如适用于甲烷氧化偶联的催化剂。图形抽象
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来源期刊
CiteScore
5.30
自引率
16.10%
发文量
205
审稿时长
4.8 months
期刊介绍: The Journal of Material Cycles and Waste Management has a twofold focus: research in technical, political, and environmental problems of material cycles and waste management; and information that contributes to the development of an interdisciplinary science of material cycles and waste management. Its aim is to develop solutions and prescriptions for material cycles. The journal publishes original articles, reviews, and invited papers from a wide range of disciplines related to material cycles and waste management. The journal is published in cooperation with the Japan Society of Material Cycles and Waste Management (JSMCWM) and the Korea Society of Waste Management (KSWM).
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