使用纳米镍金属催化剂在水介质中选择性加氢将二氧化碳转化为甲酸并获得更高产率:通过响应面方法(RSM)优化反应参数

IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Rajeev Ranjan, Prakash Biswas and K. K. Pant
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引用次数: 0

摘要

本研究采用溶胶-凝胶法合成了一种高活性介孔纳米镍催化剂,用于在水介质中将二氧化碳选择性转化为甲酸(FA)。本研究在高压釜中进行了二氧化碳加氢反应,并采用响应面法(RSM)设定了实验条件。RSM 分析采用了三因素、单响应和五级中央复合设计(CCD),并结合了可取性方法。实验表明,在优化的反应条件(200 oC,60 bar)下,甲酸产率显著提高(2245 μmol g-1 h-1),催化剂选择性达到 100%。在水介质和非镍纳米金属催化剂存在的情况下,获得的翻转数(TON)约为 285,明显更高。介孔纳米镍颗粒(15-26 纳米)促进了氢分子的选择性吸附和分裂为氢自由基,氢自由基进一步与反应介质中的碳酸根离子反应。Na2CO3 起到了促进剂的作用,提高了二氧化碳的吸附和甲酸的产量。催化剂的可回收性通过五次实验得到证实,并发现甲酸的产量保持不变。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Selective hydrogenation of CO2 to formic acid with higher yield in an aqueous medium with a nano-nickel-metal catalyst: reaction parameter optimization by response surface methodology (RSM)†

Selective hydrogenation of CO2 to formic acid with higher yield in an aqueous medium with a nano-nickel-metal catalyst: reaction parameter optimization by response surface methodology (RSM)†

A highly active mesoporous nano-nickel catalyst was synthesized by the sol–gel method for the selective conversion of CO2 to formic acid (FA) in an aqueous medium. In this study, CO2 hydrogenation reactions were performed in a high-pressure autoclave, and the experimental conditions were set by using the response surface methodology (RSM). The RSM analysis was done using a three-factor, one-response, and five-level central composite design (CCD) integrated with the desirability approach. Experiments revealed that under the optimized reaction conditions (200 °C, 60 bar), the obtained formic acid yield was significantly high (2245 μmol g−1 h−1) with 100% catalyst selectivity. The obtained turnover number (TON) was ∼285, significantly higher in an aqueous medium and the presence of a non-noble nickel nano-metal catalyst. Mesoporous nano nickel particles (15–26 nm) facilitated the selective adsorption and splitting of hydrogen molecules to hydrogen radicals, which further reacted with the carbonate ions present in the reaction medium. Na2CO3 acted as a promoter, which enhanced the CO2 adsorption and the formic acid yield. The catalyst recyclability was confirmed by performing the experiments five times and a constant yield of formic acid was found.

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来源期刊
Reaction Chemistry & Engineering
Reaction Chemistry & Engineering Chemistry-Chemistry (miscellaneous)
CiteScore
6.60
自引率
7.70%
发文量
227
期刊介绍: Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society. From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.
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