Synergistic decomposition of H2S into H2 by Ni3S2 over ZrO2 support via a sulfur looping scheme with CO2 enabled carrier regeneration

Jangam, Kalyani; Joshi, Anuj; Chen, Yu‐Yen; Mahalingam, Shailaja; Sunny, Ashin A.; Fan, Liang‐Shih

doi:10.1016/j.cej.2021.131815

Cited by 20 publications

(11 citation statements)

References 64 publications

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“…Employing the Ni 3 S 2 as the active component, high-performance catalysts with ZrO 2 and MgAl 2 O 4 supports were developed for the splitting of H 2 S into H 2 . 196 Compared with Ni 3 S 2 -MgAl, the Ni 3 S 2 -Zr presented a sulfur uptake of 100% at a high GHSV of 5000 h −1 during continuous 10 redox cycles (Figure 6). The DFT calculation revealed that MgAl 2 O 4 only acted as an inert support, while the ZrO 2 carrier showcased bifunctional characteristics.…”

Section: Catalytic Splitting Of H 2 Smentioning

confidence: 98%

“…Ni 3 S 2 presented an equilibrium H 2 yield of 80% while that of NiS was only 10%. Employing the Ni 3 S 2 as the active component, high-performance catalysts with ZrO 2 and MgAl 2 O 4 supports were developed for the splitting of H 2 S into H 2 . Compared with Ni 3 S 2 -MgAl, the Ni 3 S 2 -Zr presented a sulfur uptake of 100% at a high GHSV of 5000 h –1 during continuous 10 redox cycles (Figure ).…”

Section: Catalytic Splitting Of H2smentioning

confidence: 99%

Section: Catalytic Splitting Of H2smentioning

confidence: 99%

See 2 more Smart Citations

Advances in Resources Recovery of H₂S: A Review of Desulfurization Processes and Catalysts

Zheng,

Lei,

Wang

et al. 2023

ACS Catal.

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Hydrogen sulfide (H 2 S) is a notorious and lethal gas widely generated in human economic activities and natural occurrences. The growing demand for pollution control makes it vital for the development of efficient processes to remove and convert H 2 S into high-valued products. As such, diversified technologies have been extensively explored, including H 2 S splitting, selective oxidation of H 2 S, and simultaneous conversion of H 2 S and CO 2 . In this review, the state-of-the-art processes for H 2 S conversion and utilization are reviewed. The potentials of various value-added products from H 2 S utilization, such as H 2 , syngas, COS, CH 3 SH, and other sulfur-containing fine chemicals are elucidated in detail. Notably, the traditional and emerging materials for H 2 S removal, mainly including metal oxide catalysts and carbon-based materials are also overviewed in this review. In addition, the catalytic mechanisms for these desulfurization reactions are also briefly discussed. Lastly, perspectives are given on the viability and technological gaps for each technology and corresponding catalysts.

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Section: Catalytic Splitting Of H 2 Smentioning

confidence: 98%

Section: Catalytic Splitting Of H2smentioning

confidence: 99%

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Advances in Resources Recovery of H₂S: A Review of Desulfurization Processes and Catalysts

Zheng,

Lei,

Wang

et al. 2023

ACS Catal.

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“…Rising concerns regarding the detrimental impact of fossil fuel-based carbon dioxide (CO 2 ) emissions on the environment have necessitated efforts to shift to carbon-neutral and carbon-negative feedstocks. , However, the growing chemical demands because of the rising population and increasing industrialization have resulted in the current chemical economy being dominated by fossil fuels due to their low cost. − Thus, there is a huge thrust in upgrading various domestic and unconventional sources such as biomass, biogas, and hydrogen sulfide (H 2 S) − to generate hydrogen (H 2 ), syngas, or liquid biofuels, in a cost-effective, carbon-free, or carbon-negative aspect. Lignocellulosic biomass is an attractive feedstock that is increasingly looked at to be transformed into valuable products. , As biomass is derived from agricultural and forest residues, it is abundant and cheap, and can be considered to be almost carbon neutral as it utilizes atmospheric CO 2 for its growth. , Moreover, if carbon capture methodologies are applied to biomass processing, then net CO 2 -negative products are also viable.…”

Section: Introductionmentioning

confidence: 99%

Thermodynamic Evaluation of the Cross-Current Moving-Bed Chemical Looping Configuration for Efficient Conversion of Biomass to Syngas

Joshi,

Falascino

et al. 2023

Energy Fuels

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The rising chemical demand and its associated concern of climate change have put an impetus on converting diverse domestic sources to valuable products in a decarbonized manner. Lignocellulosic biomass, a viable feedstock, is garnering significant attention as a sustainable alternative to fossil fuels. However, challenges in handling biomass feed variability and effectively processing its char and tar contents have hampered its commercial deployment. However, the chemical looping-based biomass-to-syngas (BTS) technology being developed by The Ohio State University is among the most promising technologies for industrial biomass reforming. It utilizes proprietary iron oxide particles in a cocurrent moving-bed reactor, leveraging the flow dynamics to transform biomass to syngas, and has been proven to be more efficient than conventional processes. However, this cocurrent system suffers from a thermodynamic barrier, inhibiting the syngas yield. To overcome this barrier, a novel chemical looping crosscurrent system is developed and investigated through detailed thermodynamic ASPEN studies after accounting for practical constraints. The barrier in the cocurrent system can be attributed to the equilibrium between exiting syngas and solid streams, which limits the oxidation of oxygen carriers. The cross-current reactor system overcomes this issue by shifting the exit of the syngas stream to the middle of the reactor, thus not allowing the exiting syngas and solid streams to be in equilibrium and creating a cocurrent section above the syngas exit and a countercurrent section below it. Thermodynamic simulations conducted under autothermal conditions reveal that the cocurrent and cross-current systems perform similarly with steam and CO 2 co-injection. However, under an isothermal condition, which is now feasible with cheaper and sustainable heating methods, the cross-current system achieves ∼34% higher syngas yield over the cocurrent system (∼0.074 in cross-current compared to ∼0.055 in cocurrent) for both steam and CO 2 co-injection. The findings from this study justify the scale-up of the cross-current system and provide system-level insights into biomass valorization.

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“…These arrangements encompass a range of processes such as combustion, reforming, hydrogen generation, dry reforming, and oxidative coupling . While the realm of chemical looping applications extends beyond these aforementioned processes, including hydrogen sulfide abatement and ammonia production, this Account primarily highlights its role in CO 2 utilization. Chemical looping offers several advantages over conventional methods, including inherent product separation, enhanced process flexibility, autothermal characteristics, and simple scalability, positioning it as a promising technology. − Notably, under specific conditions, our chemical looping gasification technique can generate high-quality syngas utilizing CO 2 as a partial substitute to steam, rendering the process CO 2 negative. , …”

Section: Introductionmentioning

confidence: 99%

Nanoscaled Oxygen Carrier-Driven Chemical Looping for Carbon Neutrality: Opportunities and Challenges

Sunny,

Meng,

Kumar

et al. 2023

Acc. Chem. Res.

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Conspectus Climate change poses unprecedented challenges, demanding efforts toward innovative solutions. Amid these efforts, chemical looping stands out as a promising strategy, attracting attention for its CO2 capture prowess and versatile applications. The chemical looping approach involves fragmenting a single reaction, often a redox reaction, into multiple subreactions facilitated by a carrier, frequently a metal oxide. This innovative method enables diverse chemical transformations while inherently segregating products, enhancing process flexibility, and fostering autothermal properties. An intriguing facet of this novel technique lies in its capacity for CO2 utilization in processes like dry reforming and gasification of carbon-based feeds such as natural gas and biomass. Central to the success of chemical looping technology is a profound understanding of the intricacies of redox chemistry within these processes. Notably, nanoscaled oxygen carriers have proven effective, characterized by their extensive surface area and customizable structure. These carriers hold substantial promise, enabling reactions under milder conditions. This Account offers a concise overview of the mechanisms, benefits, opportunities, and challenges associated with nanoscaled carriers in chemical looping applications, with a focus on CO2 utilization. We delve into the nuances of redox chemistry, shedding light on ionic diffusion and oxygen vacancytwo key elements that are crucial in designing oxygen carriers. This discussion extends to nanospecific factors such as the particle size effect and gas diffusivity. Through the application of density functional theory simulations, insights are drawn regarding the impact of nanoparticle size on syngas production in chemical looping. Interestingly, nanosized iron oxide (Fe2O3) carriers exhibit elevated syngas selectivity and constrained CO2 formation at the nanoscale. Moreover, the reactivity enhancement of mesoporous SBA-16 supported Fe2O3 over mesoporous SBA-15 supported Fe2O3 is elucidated through Monte Carlo simulations that emphasize the superiority of the 3-dimensional interconnected porous network of SBA-16 in enhancing gas diffusion, thereby amplifying reactivity compared to the 2-dimensional SBA-15. Furthermore, we explore prevalent nanoscaled carriers, focusing on their amplified performance in CO2 utilization schemes. These encompass the integration of nanoparticles with mesoporous supports to enhance surface area, the adoption of nanoscale core–shell architectures to enhance diffusion, and the dispersion of nanoscaled active sites on microsized carriers to accelerate reactant activation. Notably, our mesoporous-supported Fe2O3 nanocarrier facilitates methane dissociation and oxidation by reducing energy barriers, thereby promoting methane conversion. The Account proceeds to outline key challenges and prospects for nanoscaled carriers in chemical looping, concluding with a glance into future research directions. We also shine a spotlight on our research group’s efforts in innovati...

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Synergistic decomposition of H2S into H2 by Ni3S2 over ZrO2 support via a sulfur looping scheme with CO2 enabled carrier regeneration

Cited by 20 publications

References 64 publications

Advances in Resources Recovery of H₂S: A Review of Desulfurization Processes and Catalysts

Advances in Resources Recovery of H₂S: A Review of Desulfurization Processes and Catalysts

Thermodynamic Evaluation of the Cross-Current Moving-Bed Chemical Looping Configuration for Efficient Conversion of Biomass to Syngas

Nanoscaled Oxygen Carrier-Driven Chemical Looping for Carbon Neutrality: Opportunities and Challenges

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Synergistic decomposition of H2S into H2 by Ni3S2 over ZrO2 support via a sulfur looping scheme with CO2 enabled carrier regeneration

Cited by 20 publications

References 64 publications

Advances in Resources Recovery of H2S: A Review of Desulfurization Processes and Catalysts

Advances in Resources Recovery of H2S: A Review of Desulfurization Processes and Catalysts

Thermodynamic Evaluation of the Cross-Current Moving-Bed Chemical Looping Configuration for Efficient Conversion of Biomass to Syngas

Nanoscaled Oxygen Carrier-Driven Chemical Looping for Carbon Neutrality: Opportunities and Challenges

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Resources

About

Advances in Resources Recovery of H₂S: A Review of Desulfurization Processes and Catalysts

Advances in Resources Recovery of H₂S: A Review of Desulfurization Processes and Catalysts