Holey carbon nanomeshes with atomically Cu–N4 active sites for efficient carbonyl sulfide catalytic hydrolysis

Lei, Ganchang; Liu, Dong; Ma, Yunjian; Wang, Shiping; Zhan, Yingying; Jiang, Lilong

doi:10.1016/j.carbon.2023.118039

Cited by 14 publications

(2 citation statements)

References 41 publications

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“…The pyridinic N concentration and structural defects have been discovered to impact H 2 S selective oxidation performance. , Kan’s findings further imply that N sites, particularly pyridinic N sites with basicity, play an critical role in the interaction of H 2 S with the nitrogen species on the carbon framework. This is because the pyridinic N atoms with additional lone-pair electrons enhance the electron-donating capacity of N-doped carbon to have more Lewis basic sites, which promotes the adsorption, activation, and dissociation of H 2 S, resulting in the rapid conversion of H 2 S to elemental S. − In addition, carbon nitride (C 3 N 4 ) or single-atom doped carbon (SAC) catalysts , are also proven as efficient H 2 S selective oxidation catalysts. It revealed that the abundant N species in C 3 N 4 as well as the special coordination between metal atom and nitrogen species in SAC could promote the ability of adsorption and dissociation for H 2 S molecules.…”

Section: Introductionmentioning

confidence: 99%

Manipulation of Waste-Activated Carbon Absorbers as Efficient Carbocatalysts for H₂S Selective Oxidation

Wang,

Liu,

Shan

et al. 2024

Ind. Eng. Chem. Res.

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Carbon-based catalysts have been widely reported as efficient metal-free catalysts for the selective oxidation of hydrogen sulfide (H 2 S). Waste-activated carbon adsorbed with saturated VOCs (i.e., styrene) has a complicated composition, and its recycling and reuse have become a major global concern due to the catastrophic environmental damage that wrong treatment may create. Here, we show a simple, green, and low-energy solvent-free method to prepare N-doped porous carbocatalysts for selective oxidation of H 2 S by direct carbonization of waste-activated carbon adsorbed with saturated VOCs mixed with melamine. The assynthesized catalysts (N@AC-T) have high specific surface areas and a significant number of active pyridinic N sites. The optimized N-doped carbon (N@AC-700) catalyst exhibits competitive H 2 S selective oxidation activity (H 2 S conversion of 96.2% and sulfur formation rate of 225 g sulfur •kg cat.−1 •h −1 at 190 °C) and superior stability (around 50 h) and water vapor resistance. Furthermore, the monolithic carbon catalysts prepared by using a biomass binder also present excellent desulfurization performance (H 2 S conversion >90% at 190 °C). The excellent catalytic performance was shown by a series of characterization results to be related to the combined effect of specific surface areas and the pyridinic N active sites. This work aims to design and prepare efficient N-doped carbon desulfurization catalysts for high potential industrial applications by rationally recycling and reusing waste carbon through a green and nonpolluting solvent-free method.

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Section: Introductionmentioning

confidence: 99%

Manipulation of Waste-Activated Carbon Absorbers as Efficient Carbocatalysts for H₂S Selective Oxidation

Wang,

Liu,

Shan

et al. 2024

Ind. Eng. Chem. Res.

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“…Owing to largely growing demand for natural gas, the effective desulfurization is attracting increasing research interests from industrial and academic fields . Techniques for the removal of sulfide substances from natural gas include absorption, catalytic conversion, adsorption, membrane separation, and others . Selective dissolution-driven absorption has been most widely applied in the purification of natural gas in a mature and cost-effective manner .…”

Section: Introductionmentioning

confidence: 99%

Unveiling the Quantitative Relationships between Electron Distribution and Steric Hindrance of Organic Amines and Their Reaction Rates with Carbonyl Sulfur: A Theoretical Calculation Investigation

Liu,

Chen,

Guo

et al. 2023

J. Phys. Chem. A

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The removal of carbonyl sulfide (COS) commonly contained in natural gas is of great significance but still very challenging via a widely employed absorption process due to its low reactivity and solubility in various commercial solvents. Artificial intelligence (AI) is playing an increasingly important role in the exploration of desulfurization solvents. However, practically feasible AI models still lack a thorough understanding of the reaction mechanisms. Machine learning (ML) models established on chemical mechanisms exhibit enhanced chemical interpretability and prediction performance. In this study, we constructed a series of solvent molecules with varying functional groups, including linear aliphatic amines, cyclic aliphatic amines, and aromatic amines and proposed a three-step reaction pathway to dissect the effects of charge and steric hindrance of different substituents on their reaction rates with COS. Chemical descriptors, based on electrostatic potential (ESP), average local ionization energy (ALIE) theory, Hirshfeld charges, and Fukui functions, were used to correlate and predict the electrophilic reactivity of amine groups with COS. Substituents influence the reaction rate by changing the attraction interaction of amine groups to COS molecules and the electron rearrangement in the electrophilic reaction. Furthermore, they have more pronounced steric effects on the reaction rate in the linear amines. The descriptors N_ALIE and q(N) were found to be crucial in predicting the reactivity of amine groups with COS. Present study provides a comprehensive understanding of the reaction mechanisms of COS with amine compounds, offers specific chemical principles for the development of chemistry-driven ML models, sheds light on other types of electrophilic reactions occurring on amine and phosphine groups, and guides the development of chemical solvents in gas absorption processes.

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Preparation of ZrO2/γ-Al2O3 albumen type catalyst and its catalytic performance for carbonyl sulfide hydrolysis

Zhang,

Chen,

Zhang

et al. 2024

Appl. Phys. A

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Holey carbon nanomeshes with atomically Cu–N4 active sites for efficient carbonyl sulfide catalytic hydrolysis

Cited by 14 publications

References 41 publications

Manipulation of Waste-Activated Carbon Absorbers as Efficient Carbocatalysts for H₂S Selective Oxidation

Manipulation of Waste-Activated Carbon Absorbers as Efficient Carbocatalysts for H₂S Selective Oxidation

Unveiling the Quantitative Relationships between Electron Distribution and Steric Hindrance of Organic Amines and Their Reaction Rates with Carbonyl Sulfur: A Theoretical Calculation Investigation

Preparation of ZrO2/γ-Al2O3 albumen type catalyst and its catalytic performance for carbonyl sulfide hydrolysis

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Holey carbon nanomeshes with atomically Cu–N4 active sites for efficient carbonyl sulfide catalytic hydrolysis

Cited by 14 publications

References 41 publications

Manipulation of Waste-Activated Carbon Absorbers as Efficient Carbocatalysts for H2S Selective Oxidation

Manipulation of Waste-Activated Carbon Absorbers as Efficient Carbocatalysts for H2S Selective Oxidation

Unveiling the Quantitative Relationships between Electron Distribution and Steric Hindrance of Organic Amines and Their Reaction Rates with Carbonyl Sulfur: A Theoretical Calculation Investigation

Preparation of ZrO2/γ-Al2O3 albumen type catalyst and its catalytic performance for carbonyl sulfide hydrolysis

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Manipulation of Waste-Activated Carbon Absorbers as Efficient Carbocatalysts for H₂S Selective Oxidation

Manipulation of Waste-Activated Carbon Absorbers as Efficient Carbocatalysts for H₂S Selective Oxidation