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通过直接手动研磨策略制备的用于甲烷高效催化燃烧的氢氧化镍纳米片

Nickel Hydroxide Nanosheets Prepared by a Direct Manual Grinding Strategy for High-Efficiency Catalytic Combustion of Methane.

作者信息

Chen Kun, Li Wenzhi, Guo Ge, Zhu Chen, Wu Wenjian, Yuan Liang

机构信息

Laboratory of Basic Research in Biomass Conversion and Utilization, University of Science and Technology of China, Hefei 230026, PR China.

Institute of Energy, Hefei Comprehensive National Science Center, Hefei 230031, PR China.

出版信息

ACS Omega. 2022 Mar 4;7(10):8536-8546. doi: 10.1021/acsomega.1c06348. eCollection 2022 Mar 15.

Abstract

Nickel hydroxide nanosheets were prepared by a very simple direct manual grinding strategy and then calcined at 200, 300, 400, and 500°. The synthesized samples were tested in lean methane (1.0% CH, air balanced) catalytic combustion and subjected to a series of physical and chemical characterizations. The sample calcined at 200 °C (Ni(OH)-200) presented a typical nanosheet structure and the best methane catalytic activity in all the samples, which can completely catalyze methane at 400 °C. The crystal structure changed from β-Ni(OH) to NiO at a calcination temperature of 300 °C. The β-Ni(OH) nanosheets began to partially agglomerate into nanoparticles at 400 °C and almost transformed into nanoparticles at 500 °C. Interestingly, the original nanosheet samples Ni(OH)-200 and NiO-300 still maintained their morphology and structure although they all went through an activity test at 500 °C in a 1.0% CH atmosphere, which proves that the calcination of nanosheets in a CH atmosphere tended to maintain their nanosheet morphology compared with calcination in the air. Furthermore, through the activity test, X-ray photoelectron spectroscopy results, TPx, and in situ DRIFTS characterization, it was proved that the hydroxyl groups on the Ni(OH)-200 and NiO nanosheets were beneficial to the dissociation of methane on the catalyst surface, and the nanosheet structure was also prone to generating more active adsorbed oxygen, so the activation energy of methane was lowered. A methane catalytic mechanism on the Ni(OH) nanosheets and NiO nanoparticles was proposed, which further proved the key role of hydroxyl groups in methane combustion.

摘要

通过非常简单的直接手动研磨策略制备了氢氧化镍纳米片,然后在200、300、400和500℃下进行煅烧。对合成的样品进行了贫甲烷(1.0% CH₄,空气平衡)催化燃烧测试,并进行了一系列物理和化学表征。在200℃煅烧的样品(Ni(OH)₂-200)呈现出典型的纳米片结构,并且在所有样品中具有最佳的甲烷催化活性,在400℃时能够完全催化甲烷。在300℃的煅烧温度下,晶体结构从β-Ni(OH)₂转变为NiO。β-Ni(OH)₂纳米片在400℃时开始部分团聚成纳米颗粒,在500℃时几乎转变为纳米颗粒。有趣的是,尽管原始的纳米片样品Ni(OH)₂-200和NiO-300在1.0% CH₄气氛中于500℃都经历了活性测试,但它们仍然保持了其形态和结构,这证明与在空气中煅烧相比,在CH₄气氛中煅烧纳米片倾向于保持其纳米片形态。此外,通过活性测试、X射线光电子能谱结果、TPx和原位漫反射红外傅里叶变换光谱表征,证明了Ni(OH)₂-200和NiO纳米片上的羟基有利于甲烷在催化剂表面的解离,并且纳米片结构也易于产生更多的活性吸附氧,从而降低了甲烷的活化能。提出了Ni(OH)₂纳米片和NiO纳米颗粒上的甲烷催化机理,进一步证明了羟基在甲烷燃烧中的关键作用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a234/8928554/5773179f46cd/ao1c06348_0008.jpg

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