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Upgrading heterogeneous Ni catalysts with thiol modification.

ABSTRACT: Precious metal catalysts are the cornerstone of many industrial processes. Replacing precious metal catalysts with earth-abundant metals is one of key challenges for the green and sustainable development of chemical industry. We report in this work a surprisingly effective strategy toward the development of cost-effective, air-stable, and efficient Ni catalysts by simple surface modification with thiols. The as-prepared catalysts exhibit unprecedentedly high activity and selectivity in the reductive amination of aldehydes/ketones. The thiol modification can not only prevent the deep oxidation of Ni surface to endow the catalyst with long shelf life in air but can also allow the reductive amination to proceed via a non-contact mechanism to selectively produce primary amines. The catalytic performance is far superior to that of precious and non-precious metal catalysts reported in the literature. The wide application scope and high catalytic performance of the developed Ni catalysts make them highly promising for the low-cost, green production of high-value amines in chemical industry.

SUBMITTER: Ruan P

PROVIDER: S-EPMC9830375 | biostudies-literature | 2023 Jan

REPOSITORIES: biostudies-literature

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Upgrading heterogeneous Ni catalysts with thiol modification.

Ruan Pengpeng P Chen Bili B Zhou Qin Q Zhang Hansong H Wang Yahao Y Liu Kunlong K Zhou Wenting W Qin Ruixuan R Liu Zhi Z Fu Gang G Zheng Nanfeng N

Innovation (Cambridge (Mass.)) 20221214 1

Precious metal catalysts are the cornerstone of many industrial processes. Replacing precious metal catalysts with earth-abundant metals is one of key challenges for the green and sustainable development of chemical industry. We report in this work a surprisingly effective strategy toward the development of cost-effective, air-stable, and efficient Ni catalysts by simple surface modification with thiols. The as-prepared catalysts exhibit unprecedentedly high activity and selectivity in the reduc ...[more]

PMID: 36636490

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Project description:In this study, Nickel oxide-based catalysts (NixOx) were synthesized and used for the in-situ upgrading process of heavy crude oil (viscosity 2157 mPa·s, and API gravity of 14.1° at 25 °C) in aquathermolysis conditions for viscosity reduction and heavy oil recovery. All characterizations of the obtained nanoparticles catalysts (NixOx) were performed through Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM), Atomic Force Microscopy (AFM), X-Ray and Diffraction (XRD), and ASAP 2400 analyzer from Micromeritics (USA), methods. Experiments of catalytic and non-catalytic upgrading processes were carried out in a discontinuous reactor at a temperature of 300 °C and 72 bars for 24 h and 2% of catalyst ratio to the total weight of heavy crude oil. XRD analysis revealed that the use of nanoparticles of NiO significantly participated in the upgrading processes (by desulfurization) where different activated form catalysts were observed, such as α-NiS, β-NiS, Ni3S4, Ni9S8, and NiO. The results of viscosity analysis, elemental analysis, and 13C NMR analysis revealed that the viscosity of heavy crude oil decreased from 2157 to 800 mPa·s, heteroatoms removal from heavy oil ranged from S-4.28% to 3.32% and N-0.40% to 0.37%, and total content of fractions (ΣC8-C25) increased from 59.56% to a maximum of 72.21%, with catalyst-3 thank to isomerization of normal and cyclo-alkanes and dealkylation of lateral chains of aromatics structures, respectively. Moreover, the obtained nanoparticles showed good selectivity, promoting in-situ hydrogenation-dehydrogenation reactions, and hydrogen redistribution over carbons (H/C) is improved, ranging from 1.48 to a maximum of 1.77 in sample catalyst-3. On the other hand, the use of nanoparticle catalysts have also impacted the hydrogen production, where the H2/CO provided from the water gas shift reaction has increased. Nickel oxide catalysts have the potential for in-situ hydrothermal upgrading of heavy crude oil because of their great potential to catalyze the aquathermolysis reactions in the presence of steam.

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Upgrading heterogeneous Ni catalysts with thiol modification.

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Upgrading heterogeneous Ni catalysts with thiol modification.

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