Hydrothermal conversion of carbon dioxide into formate with the aid of zerovalent iron: the potential of a two-step approach

Author:

Michiels K.12345,Peeraer B.12345,Van Dun W.12345,Spooren J.12345,Meynen V.678910

Affiliation:

1. Waste Recycling Technologies

2. Sustainable Materials Management

3. Flemish Institute for Technological Research

4. VITO N.V.

5. 2400 Mol

6. Laboratory of Adsorption and Catalysis

7. Department of Chemistry

8. University of Antwerp

9. UAntwerp

10. 2610 Wilrijk

Abstract

Our research focuses on the hydrothermal conversion of carbon dioxide into formate with the aid of zerovalent iron. Conventionally, a one-step approach is applied wherein both (i) the production of hydrogen gas, through the oxidation of zerovalent iron in an aqueous medium and (ii) the conversion of carbon dioxide with this hydrogen gas into formate/formic acid, are performed under the same reaction conditions at a temperature of approximately 300 °C. Until now, the yields of formate/formic acid mentioned in the literature are, in the absence of a catalytic substance, low (13.5%). Recently, we developed a hydrothermal hydrogen gas production method based on the oxidation of zerovalent iron and performed under mild conditions (temperature of 160 °C). This synthesis method produces hydrogen gas with a high purity (>99 mol%) and a significant yield (approximately 80 mol%). These experimental results suggested that the optimal hydrothermal reaction conditions for the production of hydrogen gas and the conversion of carbon dioxide, are strongly different in case of applying zerovalent iron as the reducing agent. Therefore, this paper studies the potential of a two-step approach to enhance the carbon conversion yields. The first step is the production of hydrogen gas via the developed method at 160 °C. The second step is the conversion of carbon dioxide at higher temperatures (250–350 °C). This study reveals that the solubility of hydrogen gas into the aqueous solution is a key parameter in order to achieve a high amount of carbon conversion. Therefore, a high temperature, the degree of filling and the initial hydrogen gas amount are necessary to successfully perform the carbon dioxide conversion step with high carbon conversion yields. Applying these insights have led to the experimental observation that via a two-step approach the conversion of potassium hydrogen carbonate into potassium formate can be successfully performed with higher carbon conversion yields, up to 77.9 wt%, and a selectivity of at least 81% when applying a reaction temperature of 280 °C for 24 hours, a degree of filling with water of 50 vol% and an initial amount of hydrogen gas of 100 mmol.

Funder

Agentschap voor Innovatie door Wetenschap en Technologie

Publisher

Royal Society of Chemistry (RSC)

Subject

Physical and Theoretical Chemistry

Reference43 articles.

1. K. Byrappa and M.Yoshimura, in Handbook of Hydrothermal Technology, ed. W. Andrew, Elsevier, Oxford, 2nd edn, 2013

2. B. M. French , Stability Relations of Siderite, FeCO3, Determined in Controlled fO2 Atmospheres, Document X-644-70-102, Goddard Space Flight Center, Planetology Branch, NASA, Greenbelt, MD, 1970

3. Hydrothermal Simulation Experiments as a Tool for Studies of the Origin of Life on Earth and Other Terrestrial Planets: A Review

4. Abiotic Synthesis of Organic Compounds in Deep-Sea Hydrothermal Environments

5. Hydrothermal processing of materials: past, present and future

同舟云学术

1.学者识别学者识别

2.学术分析学术分析

3.人才评估人才评估

"同舟云学术"是以全球学者为主线,采集、加工和组织学术论文而形成的新型学术文献查询和分析系统,可以对全球学者进行文献检索和人才价值评估。用户可以通过关注某些学科领域的顶尖人物而持续追踪该领域的学科进展和研究前沿。经过近期的数据扩容,当前同舟云学术共收录了国内外主流学术期刊6万余种,收集的期刊论文及会议论文总量共计约1.5亿篇,并以每天添加12000余篇中外论文的速度递增。我们也可以为用户提供个性化、定制化的学者数据。欢迎来电咨询!咨询电话:010-8811{复制后删除}0370

www.globalauthorid.com

TOP

Copyright © 2019-2024 北京同舟云网络信息技术有限公司
京公网安备11010802033243号  京ICP备18003416号-3