Development of composite microwave catalysts (ABSx/CNTs, A = Co, B = Ni, Mo) for the highly effective direct decomposition of H2S into H2 and S

Luo, Mide; Zhou, Jicheng; Xu, Wentao; Chen, Jianan; Xiang, Min; Peng, Kang

doi:10.1016/j.fuel.2020.118729

Cited by 17 publications

(4 citation statements)

References 71 publications

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“…Fortunately, it has been reported that the higher oxidation state of Fe sites favors the dissociation of OH* intermediates (the ratedetermining step for ORR catalyzed by FeN 4 ). [21] According to this evidence, the charge separation may weaken the adsorption strength of OH* intermediates and increase the overall electrocatalytic activity.…”

Section: Strong Oxygen Adsorption On the G/cnt Interfacementioning

confidence: 94%

“…We report a one-step microwave-assisted process to fabricate nitrogen-coordinated single-atom iron on graphene/CNT hybrid electrocatalysts (the as-prepared catalyst is denoted FeNG/CNT), that has a high performance for SWBs especially under lean-oxygen seawater, in which Pt/C catalyst shows a very low ORR response. The CNTs (microwave susceptor) strongly absorb the microwave irradiation, [21] and at the same time the used graphene oxide was reduced (the reduced graphene oxide denoted as rGO). The atomic Fe catalyst was stabilized and π-π interactions between the CNTs and graphene sheets were achieved.…”

Section: Introductionmentioning

confidence: 99%

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An Oxygenophilic Atomic Dispersed FeNC Catalyst for Lean‐Oxygen Seawater Batteries

Meng

Zhang

et al. 2021

Advanced Energy Materials

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A constant energy supply is crucial for the exploration of deep‐sea extreme environments, and a self‐powered energy conversion device is ideal for this situation. Dissolved‐oxygen seawater batteries (SWBs) that generate electricity by reducing the dissolved oxygen are promising candidates but the ultralow oxygen concentration in deep sea limits the reaction kinetics. As a result, oxygenophilic electrocatalysts for lean‐oxygen conditions are urgently needed. A microwave heating method is reported that achieves the ultrafast synthesis of atomic dispersed FeNC catalyst (FeNgraphene (G)/carbon nanotube (CNT)), which possesses high activity and strong oxygenophilic interface between graphene and CNTs. DFT calculations and experimental results both show that the high oxygenophilicity is due to the double‐adsorption sites on the G/CNT interface, and the high activity FeN4 active sites is caused by the charge separation. FeNG/CNT catalysts have an outstanding oxygen reduction reaction (ORR) performance in both O2‐saturated alkaline medium and neutral seawater with half‐wave potentials (E1/2) of 0.929 and 0.704 V, respectively, far better than commercial Pt/C. A SWB shows excellent performance in lean‐oxygen seawater (≈0.4 mg L−1), with a discharge voltage of 1.18 V at 10 mA cm−2. These results suggest a critical role for oxygenophilic catalyst specifically for SWBs under lean‐oxygen conditions.

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Section: Strong Oxygen Adsorption On the G/cnt Interfacementioning

confidence: 94%

Section: Introductionmentioning

confidence: 99%

An Oxygenophilic Atomic Dispersed FeNC Catalyst for Lean‐Oxygen Seawater Batteries

Meng

Zhang

et al. 2021

Advanced Energy Materials

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“…Furthermore, microwave effect is divided into thermal effect and nonthermal effect to explain some properties that cannot be realized by heating alone. There are still many disputes about the existence of microwave nonthermal effect. − In the experiment, the microwave nonthermal effect cannot be separated from the thermal effect because of the different heating mechanism that microwave and traditional heating cannot construct the same temperature field. In theory, nonthermal effect cannot be properly defined using molecular mechanics simulations .…”

Section: Introductionmentioning

confidence: 99%

Microwave Hotspots: Thermal Nonequilibrium Dynamics from the Perspective of Quantum States

2021

J. Phys. Chem. A

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The observed microwave effects include thermal effect, superheating or hotspots, and selective heating. These phenomena are almost impossible in classical heating, and the existence of nonthermal effect is still a controversial topic. Hotspot effect is a phenomenon that is often observed in microwave-assisted reaction and is significantly different from the traditional heating reaction. We use the quantum-state specified master equation model of microwave-assisted reaction proposed in 2016 to study the possible mechanism of microwave hotspots. We divide the hotspots into space hotspots and intramolecular hotspots, which correspond to thermal conduction and luminous behavior, respectively. For the model system in the microwave field, the microwave hotspot cannot be generated at a very low temperature of 100 K, and it is possible to generate the microwave hotspot above 300 K. Moreover, the probability of generating the microwave hotspot at 500 K is about 75 times higher than that at 350 K. The appearance of this nonlinear phenomenon is related to the uneven distribution of temperature and microwave intensity in the macroscopic level and directly related to the nonequilibrium behavior caused by microwave absorption in the quantum-state level. It is suggested that microwave hotspots can be induced by heating the given regions in the reaction vessel in advance. In addition, the formation of intramolecular hotspots can also be induced by pre-exciting the local groups in specific molecules.

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“…However, the direct decomposition of H 2 S is a highly endothermic process (with a reaction enthalpy of +169.4 kJ/mol) with limited thermodynamic conversion at temperatures below 1000 K . Aside from thermocatalytic efforts for direct H 2 S decomposition, , there have been attempts to achieve faster kinetic rates at milder temperatures using electrocatalytic, , photocatalytic, − plasma-induced, and microwave-assisted approaches. , Chemical looping , has also been implemented to circumvent the thermodynamic limitation of this reaction. While these studies represent valuable progress toward the direct decomposition of H 2 S at milder temperatures, difficulties with scale-up due to the energy source or the catalyst are still major challenges.…”

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confidence: 99%

Direct H₂S Decomposition by Plasmonic Photocatalysis: Efficient Remediation plus Sustainable Hydrogen Production

et al. 2022

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Plasmonic metal nanostructures have garnered rapidly increasing interest as heterogeneous photocatalysts, facilitating chemical bond activation and overcoming the high energy demands of conventional thermal catalysis. Here we report the highly efficient plasmonic photocatalysis of the direct decomposition of hydrogen sulfide into hydrogen and sulfur, an alternative to the industrial Claus process. Under visible light illumination and with no external heat source, up to a 20-fold reactivity enhancement compared to thermocatalysis can be observed. The substantially enhanced reactivity can be attributed to plasmon-mediated hot carriers (HCs) that modify the reaction energetics. With a shift in the rate-determining step of the reaction, a new reaction pathway is made possible with a lower apparent reaction barrier. Light-driven one-step decomposition of hydrogen sulfide represents an exciting opportunity for simultaneous high-efficiency hydrogen production and low-temperature sulfur recovery, important in many industrial processes.

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Development of composite microwave catalysts (ABSx/CNTs, A = Co, B = Ni, Mo) for the highly effective direct decomposition of H2S into H2 and S

Cited by 17 publications

References 71 publications

An Oxygenophilic Atomic Dispersed FeNC Catalyst for Lean‐Oxygen Seawater Batteries

An Oxygenophilic Atomic Dispersed FeNC Catalyst for Lean‐Oxygen Seawater Batteries

Microwave Hotspots: Thermal Nonequilibrium Dynamics from the Perspective of Quantum States

Direct H₂S Decomposition by Plasmonic Photocatalysis: Efficient Remediation plus Sustainable Hydrogen Production

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Development of composite microwave catalysts (ABSx/CNTs, A = Co, B = Ni, Mo) for the highly effective direct decomposition of H2S into H2 and S

Cited by 17 publications

References 71 publications

An Oxygenophilic Atomic Dispersed FeNC Catalyst for Lean‐Oxygen Seawater Batteries

An Oxygenophilic Atomic Dispersed FeNC Catalyst for Lean‐Oxygen Seawater Batteries

Microwave Hotspots: Thermal Nonequilibrium Dynamics from the Perspective of Quantum States

Direct H2S Decomposition by Plasmonic Photocatalysis: Efficient Remediation plus Sustainable Hydrogen Production

Contact Info

Product

Resources

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Direct H₂S Decomposition by Plasmonic Photocatalysis: Efficient Remediation plus Sustainable Hydrogen Production