Molecular-level heavy petroleum hydrotreating modeling and comparison with high-resolution mass spectrometry

Guan, Dong; Chen, Zhengyu; Chen, Xiu; Zhang, Ying; Qi, Qiuyan; Shi, Quan; Zhao, Suoqi; Chen, Xu; Zhang, Linzhou

doi:10.1016/j.fuel.2021.120792

Cited by 26 publications

(31 citation statements)

References 73 publications

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“…The model results show good agreement with the bulk property data. Moreover, the predicted molecular distribution and molecular conversion regulations are consistent with the high-resolution mass spectrometry data . The authors state that they ignore molecules with extremely low content in their modeling.…”

Section: Structure–dynamic Function: Reactive Chemistrysupporting

confidence: 64%

“…In addition, this assumption applies to the bulk of asphaltene molecular structures and furthermore implies that there are no nonlinearities in the actual system introduced by multiple heteroatoms. Many metrics were obtained in this work, showing excellent agreement between modeling and measured results using the assumptions in Table ; a few results are shown here …”

Section: Structure–dynamic Function: Reactive Chemistrysupporting

confidence: 63%

“…For the heavy ends, this represents a significant challenge, in particular, because of the difficulty in accounting for asphaltene chemical structures. A methodology has been developed to yield molecular management of refining and has been applied in various ways. , In some cases, the protocol for the molecular management of refining has presumed that archipelago molecules are plentiful in asphaltenes . The success of this modeling effort to provide detailed accounting of reaction products from complex reactant mixtures of heavy ends has frequently been cited as “proof” that asphaltenes have plentiful archipelago molecular structures.…”

Section: Structure–dynamic Function: Reactive Chemistrymentioning

confidence: 99%

“…The authors state that they ignore molecules with extremely low content in their modeling. They make four assumptions about molecular structures for the heavy oils, as shown in Table …”

Section: Structure–dynamic Function: Reactive Chemistrymentioning

confidence: 99%

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Structure–Dynamic Function Relations of Asphaltenes

et al. 2021

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Asphaltene molecular and nanocolloidal structures have largely been resolved enabling development of structure–function relations of asphaltenes. Atomic force microscopy (AFM) and scanning tunneling microscopy (STM) have provided the first direct molecular structures of many asphaltenes with extension into broader distributions of petroleum pitch. These studies confirmed previous findings of dominant island architecture, moderate-sized polycyclic aromatic hydrocarbons (PAHs) with significant variability in the number and geometry of these rings. The Yen–Mullins model of centroids of molecular and nanocolloidal species of asphaltenes continues to provide foundations for thermodynamic treatment of crude oils, for both bulk and surface. Herein, these asphaltene structures are subject to the stringent test of modeling dynamic function along with static function. Recent results impact evaluation of the molecular management of heavy oil refining for the hydrotreatment process. Roughly, 25,000 reactions were considered acting on ∼17,000 molecules. Reactants and products are probed with ultrahigh-resolution mass spectrometry. In modeling, consistency is required with AFM molecular imaging results of asphaltenes. Excellent agreement is obtained between modeling and experiment, increasing accuracy and robustness. Thermodynamic treatments of asphaltenes in bulk and surface are shown within a structure–dynamic function setting. Two oilfield reservoirs are reviewed which are undergoing different diffusive processes in geologic time. The dynamic model to evaluate both reservoirs couples the simplest solution of the diffusion equation with a quasi-equilibrium state employing the Yen–Mullins model in parts distant from the diffusive process, and excellent agreement between modeling and measurement is obtained. For interfacial tension (IFT), a static model employing the simple Langmuir equation successfully treats solutions of moderate asphaltene concentrations and is consistent with AFM images of asphaltenes. A first-order dynamic correction of time evolution of the IFT can be accounted for considering some molecular polydispersity. Structure–dynamic function relations are established for asphaltenes in three very different arenas.

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Section: Structure–dynamic Function: Reactive Chemistrysupporting

confidence: 64%

Section: Structure–dynamic Function: Reactive Chemistrysupporting

confidence: 63%

Section: Structure–dynamic Function: Reactive Chemistrymentioning

confidence: 99%

“…The authors state that they ignore molecules with extremely low content in their modeling. They make four assumptions about molecular structures for the heavy oils, as shown in Table …”

Section: Structure–dynamic Function: Reactive Chemistrymentioning

confidence: 99%

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Structure–Dynamic Function Relations of Asphaltenes

et al. 2021

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“…Detailed characterization of petroleum compositions can have a significant impact on the processing/conversion of highly complex materials and the quality of related products. , The advances in analytical techniques have been, in large part, driven by the needs in composition-based modeling to guide process chemistry, to optimize and improve manufacturing operations, and to maximize the values of the raw materials. − For example, the structure-oriented lumping (SOL) modeling platform, as proposed in 1992 by Quann and Jaffe, was based on petroleum composition described as a mixture of hydrocarbon molecules using vectors of 22 structural increments. Later in 2006, Jaffe et al further expanded the SOL framework into vacuum residue (VR) by invoking a multicore concept and adding two more vectors for VO and Ni porphyrins .…”

Section: Introductionmentioning

confidence: 99%

Molecular Characterization of Heavy Petroleum by Mass Spectrometry and Related Techniques

Qian

2021

Energy Fuels

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The rapid advances in mass spectrometry and related technologies in the last two decades have revolutionized our understanding of heavy petroleum composition and greatly accelerated research and development within the oil and gas industry. Petroleum is a highly complex mixture of hydrocarbons and heteroatom-containing (S, N, O, metals, and more) hydrocarbons. Molecular composition has a significant impact on the properties of crude oils and the way they need to be handled in refining processes. In this review, the current state is highlighted, as well as progress in key areas of the molecular characterization of heavy petroleum, including separation approaches, ionization methods, high-resolution mass spectrometry, dissociation technology, and multidimensional separation mass spectrometry, including GC soft ionization mass spectrometry and ion mobility-mass spectrometry.

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A molecular kinetic model incorporating catalyst acidity for hydrocarbon catalytic cracking

et al. 2023

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This work built a molecular-level kinetic model for hydrocarbon catalytic cracking, incorporating the catalyst acidity as the parameter to estimate reaction rates. The ndecane and 1-hexene co-conversion catalytic cracking process was chosen as the studying case. The molecular reaction network was automatically generated using a computer-aided algorithm. A modified linear free energy relationship was proposed to estimate the activation energy in a complex reaction system. The kinetic parameters were initially regressed from the experimental data under several reaction conditions. On this basis, the product composition was evaluated for three catalytic cracking catalysts with different Si/Al. The Bronsted acid and Lewis acid as the key catalyst properties were correlated with kinetic parameters. The built model can calculate the product distribution, gasoline composition, and molecular distribution at different reaction conditions for different catalysts. This sensitive study shows that it will facilitate the model-based optimization of catalysts and reaction conditions according to product demands.

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Molecular-level heavy petroleum hydrotreating modeling and comparison with high-resolution mass spectrometry

Cited by 26 publications

References 73 publications

Structure–Dynamic Function Relations of Asphaltenes

Structure–Dynamic Function Relations of Asphaltenes

Molecular Characterization of Heavy Petroleum by Mass Spectrometry and Related Techniques

A molecular kinetic model incorporating catalyst acidity for hydrocarbon catalytic cracking

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