Simultaneous catalytic oxidation of nitric oxide and elemental mercury by single-atom Pd/g-C3N4 catalyst: A DFT study

Liu, Xiaoshuo; Gao, Zhengyang; Huang, Hanyu; Gao, Yan; Huang, Tianfang; Chen, Cong; Ding, Xiaobin

doi:10.1016/j.mcat.2020.110901

Cited by 21 publications

(17 citation statements)

References 81 publications

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“…Even the pure Ph-g-C 3 N 4 structure is highly distorted due to the high strain induced by delocalization of π-electrons and the existence of void spaces in the g-C 3 N 4 structure. This is consistent with previously reported results. , …”

Section: Resultssupporting

confidence: 94%

“…This large and negative value of the binding energy confirms the excellent binding between the adsorbed unit and suggests that this reaction should be exothermic. However, after considering the BSSE correction, the estimated adsorption energy remains a negative value (−1.48 eV, Table S7) and is in good accordance with the value of −1.43 eV recently reported for the adsorption of single-metal atoms on the g-C 3 N 4 surface and that of −1.61 eV for the adsorption of COOH on a g-C 3 N 4 support …”

Section: Resultssupporting

confidence: 90%

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Phenyl-Modified Carbon Nitride Quantum Nanoflakes for Ultra-Highly Selective Sensing of Formic Acid: A Combined Experimental by QCM and Density Functional Theory Study

Torad

El-Hosainy

Esmat

et al. 2021

ACS Appl. Mater. Interfaces

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Formic acid (HCOOH) is an important intermediate in chemical synthesis, pharmaceuticals, the food industry, and leather tanning and is considered to be an effective hydrogen storage molecule. Direct contact with its vapor and its inhalation lead to burns, nerve injury, and dermatosis. Thus, it is critical to establish efficient sensing materials and devices for the rapid detection of HCOOH. In the present study, we introduce a chemical sensor based on a quartz crystal microbalance (QCM) sensor capable of detecting trace amounts of HCOOH. This sensor is composed of colloidal phenyl-terminated carbon nitride (Ph-g-C3N4) quantum nanoflakes prepared using a facile solid-state method involving the supramolecular preorganization technology. In contrast to other synthetic methods of modified carbon nitride materials, this approach requires no hard templates, hazardous chemicals, or hydrothermal treatments. Comprehensive characterization and density functional theory (DFT) calculations revealed that the QCM sensor designed and prepared here exhibits enhanced detection sensitivity and selectivity for volatile HCOOH, which originates from chemical and hydrogen-bonding interactions between HCOOH and the surface of Ph-g-C3N4. According to DFT results, HCOOH is located close to the cavity of the Ph-g-C3N4 unit, with bonding to graphitic carbon and pyridinic nitrogen atoms of the nanoflake. The sensitivity of the Ph-g-C3N4-nanoflake-based QCM sensor was found to be the highest (128.99 Hz ppm–1) of the substances studied, with a limit of detection (LOD) of HCOOH down to a sub-ppm level of 80 ppb. This sensing technology based on phenyl-terminated attached-g-C3N4 nanoflakes establishes a simple, low-cost solution to improve the performance of QCM sensors for the effective discrimination of HCOOH, HCHO, and CH3COOH vapors using smart electronic noses.

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Section: Resultssupporting

confidence: 94%

Section: Resultssupporting

confidence: 90%

Phenyl-Modified Carbon Nitride Quantum Nanoflakes for Ultra-Highly Selective Sensing of Formic Acid: A Combined Experimental by QCM and Density Functional Theory Study

Torad

El-Hosainy

Esmat

et al. 2021

ACS Appl. Mater. Interfaces

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“…Lastly, SACs with graphene-like supports, such as carbon nanotubes, − C 3 N 4 , − BN, − porphyrin/phthalocyanine, ,,,, metal–organic framework (MOF), and zeolitic imidazolate framework (ZIF) generated materials, ,− also demonstrate high catalytic performance on many reactions. Their local coordination environments are more or less similar to the graphene-anchored SAs reviewed in this work.…”

Section: Discussionmentioning

confidence: 99%

Theoretical Understandings of Graphene-based Metal Single-Atom Catalysts: Stability and Catalytic Performance

et al. 2020

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Research on heterogeneous single-atom catalysts (SACs) has become an emerging frontier in catalysis science because of their advantages in high utilization of noble metals, precisely identified active sites, high selectivity, and tunable activity. Graphene, as a one-atom-thick two-dimensional carbon material with unique structural and electronic properties, has been reported to be a superb support for SACs. Herein, we provide an overview of recent progress in investigations of graphene-based SACs. Among the large number of publications, we will selectively focus on the stability of metal single-atoms (SAs) anchored on different sites of graphene support and the catalytic performances of graphenebased SACs for different chemical reactions, including thermocatalysis and electrocatalysis. We will summarize the fundamental understandings on the electronic structures and their intrinsic connection with catalytic properties of graphene-based SACs, and also provide a brief perspective on the future design of efficient SACs with graphene and graphene-like materials. CONTENTS

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“…However, the overall trend of no atmosphere is to inhibit mercury removal after the addition of H 2 O, and the increase of the H 2 O concentration may inhibit the oxidation ability of NO. NO can directly react with Hg 0 by a homogeneous oxidation reaction R2, or can be adsorbed on the surface of the mercury sorbent combined with the surface oxygen (O s ) and converted to NO 2 through R3 following the Eley–Rideal mechanism, and then react with Hg 0 by heterogeneous oxidation R4. , However, the chemical reaction kinetics of homogeneous oxidation is limited at an experimental temperature of 150 °C, and the rate of heterogeneous oxidation is higher than that of oxidation, so heterogeneous oxidation is more likely to be dominant. No matter which of the above reactions, the presence of oxygen in the process is extremely important.…”

Section: Resultsmentioning

confidence: 99%

Interference Effect of H₂O on Hg⁰ Removal by a Mercury Sorbent in an Oxyfuel-Combustion Atmosphere

Ran

Wang

et al. 2021

Ind. Eng. Chem. Res.

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The H 2 O concentration in an oxyfuel-combustion atmosphere is higher than that in a traditional combustion atmosphere, which will affect the mercury removal process. Therefore, it is necessary to carry out a research on the interference effect of H 2 O on mercury removal under an oxyfuelcombustion atmosphere. In this paper, corn straw char was modified by NH 4 Cl, and related experiments were carried out using a fixed-bed reaction system. The characterization results of the sorbent showed that the modification enhanced its physical and chemical adsorption capacities. The addition of H 2 O in a NO atmosphere was not conducive to mercury removal but could alleviate the toxicity of SO 2 on the adsorbent in a SO 2 atmosphere. The coexistence of H 2 O and NO significantly inhibited the mercury removal, but some nitrate ions were generated during the process, which slightly weakened the negative effects of H 2 O. The coexistence of low-concentration H 2 O and SO 2 would weaken the poisoning effect of SO 2 on the mercury sorbent, and high-content H 2 O would react to generate excess H 2 SO 4 to block the surface pores. SO 3 could assist Hg 0 oxidation, while H 2 O would hinder the transformation of SO 2 into SO 3 . In a HCl atmosphere, highconcentration H 2 O (20%) inhibited mercury removal, while lower-concentration H 2 O (5−15%) showed an opposite behavior. The low concentration of H 2 O did not affect the oxidation of Hg 0 by HCl, and it was accompanied by the formation of substances conducive to mercury removal. The increase of the H 2 O concentration would hinder the oxidation reaction of HCl and Hg 0 .

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Simultaneous catalytic oxidation of nitric oxide and elemental mercury by single-atom Pd/g-C3N4 catalyst: A DFT study

Cited by 21 publications

References 81 publications

Phenyl-Modified Carbon Nitride Quantum Nanoflakes for Ultra-Highly Selective Sensing of Formic Acid: A Combined Experimental by QCM and Density Functional Theory Study

Phenyl-Modified Carbon Nitride Quantum Nanoflakes for Ultra-Highly Selective Sensing of Formic Acid: A Combined Experimental by QCM and Density Functional Theory Study

Theoretical Understandings of Graphene-based Metal Single-Atom Catalysts: Stability and Catalytic Performance

Interference Effect of H₂O on Hg⁰ Removal by a Mercury Sorbent in an Oxyfuel-Combustion Atmosphere

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Simultaneous catalytic oxidation of nitric oxide and elemental mercury by single-atom Pd/g-C3N4 catalyst: A DFT study

Cited by 21 publications

References 81 publications

Phenyl-Modified Carbon Nitride Quantum Nanoflakes for Ultra-Highly Selective Sensing of Formic Acid: A Combined Experimental by QCM and Density Functional Theory Study

Phenyl-Modified Carbon Nitride Quantum Nanoflakes for Ultra-Highly Selective Sensing of Formic Acid: A Combined Experimental by QCM and Density Functional Theory Study

Theoretical Understandings of Graphene-based Metal Single-Atom Catalysts: Stability and Catalytic Performance

Interference Effect of H2O on Hg0 Removal by a Mercury Sorbent in an Oxyfuel-Combustion Atmosphere

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Product

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Interference Effect of H₂O on Hg⁰ Removal by a Mercury Sorbent in an Oxyfuel-Combustion Atmosphere