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      Reactive Capture and Conversion of CO 2 into Hydrogen over Bifunctional Structured Ce 1– x Co x NiO 3/Ca Perovskite-Type Oxide Monoliths

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          Abstract

          Carbon capture, utilization, and storage (CCUS) technologies are pivotal for transitioning to a net-zero economy by 2050. In particular, conversion of captured CO 2 to marketable chemicals and fuels appears to be a sustainable approach to not only curb greenhouse emissions but also transform wastes like CO 2 into useful products through storage of renewable energy in chemical bonds. Bifunctional materials (BFMs) composed of adsorbents and catalysts have shown promise in reactive capture and conversion of CO 2 at high temperatures. In this study, we extend the application of 3D printing technology to formulate a novel set of BFMs composed of CaO and Ce 1– x Co x NiO 3 perovskite-type oxide catalysts for the dual-purpose use of capturing CO 2 and reforming CH 4 for H 2 production. Three honeycomb monoliths composed of equal amounts of adsorbent and catalyst constituents with varied Ce 1– x Co x ratios were 3D printed to assess the role of cobalt on catalytic properties and overall performance. The samples were vigorously characterized using X-ray diffraction (XRD), energy-dispersive spectroscopy (EDS), N 2 physisorption, X-ray photoelectron spectroscopy (XPS), H 2-TPR, in situ CO 2 adsorption/desorption XRD, and NH 3-TPD. Results showed that the Ce 1– x Co x ratios— x = 0.25, 0.50, and 0.75—did not affect crystallinity, texture, or metal dispersion. However, a higher cobalt content reduced reducibility, CO 2 adsorption/desorption reversibility, and oxygen species availability. Assessing the structured BFM monoliths via combined CO 2 capture and CH 4 reforming in the temperature range 500–700 °C revealed that such differences in physiochemical properties lowered H 2 and CO yields at higher cobalt loading, leading to best catalytic performance in Ce 0.75Co 0.25NiO 3/Ca sample that achieved 77% CO 2 conversion, 94% CH 4 conversion, 61% H 2 yield, and 2.30 H 2/CO ratio at 700 °C. The stability of this BFM was assessed across five adsorption/reaction cycles, showing only marginal losses in the H 2/CO yield. Thus, these findings successfully expand the use of 3D printing to unexplored perovskite-based BFMs and demonstrate an important proof-of-concept for their use in combined CO 2 capture and utilization in H 2 production processes.

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          The role of CO2 capture and utilization in mitigating climate change

          This Perspective considers the potential mitigation contribution of carbon capture and utilization, such as chemical conversation or to enhance oil recovery. The authors find it will account for a small amount of the required total mitigation effort.
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            Pt/Cu single-atom alloys as coke-resistant catalysts for efficient C–H activation

            The recent availability of shale gas has led to a renewed interest in C-H bond activation as the first step towards the synthesis of fuels and fine chemicals. Heterogeneous catalysts based on Ni and Pt can perform this chemistry, but deactivate easily due to coke formation. Cu-based catalysts are not practical due to high C-H activation barriers, but their weaker binding to adsorbates offers resilience to coking. Using Pt/Cu single-atom alloys (SAAs), we examine C-H activation in a number of systems including methyl groups, methane and butane using a combination of simulations, surface science and catalysis studies. We find that Pt/Cu SAAs activate C-H bonds more efficiently than Cu, are stable for days under realistic operating conditions, and avoid the problem of coking typically encountered with Pt. Pt/Cu SAAs therefore offer a new approach to coke-resistant C-H activation chemistry, with the added economic benefit that the precious metal is diluted at the atomic limit.
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              Strategies for mitigation of climate change: a review

              Climate change is defined as the shift in climate patterns mainly caused by greenhouse gas emissions from natural systems and human activities. So far, anthropogenic activities have caused about 1.0 °C of global warming above the pre-industrial level and this is likely to reach 1.5 °C between 2030 and 2052 if the current emission rates persist. In 2018, the world encountered 315 cases of natural disasters which are mainly related to the climate. Approximately 68.5 million people were affected, and economic losses amounted to $131.7 billion, of which storms, floods, wildfires and droughts accounted for approximately 93%. Economic losses attributed to wildfires in 2018 alone are almost equal to the collective losses from wildfires incurred over the past decade, which is quite alarming. Furthermore, food, water, health, ecosystem, human habitat and infrastructure have been identified as the most vulnerable sectors under climate attack. In 2015, the Paris agreement was introduced with the main objective of limiting global temperature increase to 2 °C by 2100 and pursuing efforts to limit the increase to 1.5 °C. This article reviews the main strategies for climate change abatement, namely conventional mitigation, negative emissions and radiative forcing geoengineering. Conventional mitigation technologies focus on reducing fossil-based CO 2 emissions. Negative emissions technologies are aiming to capture and sequester atmospheric carbon to reduce carbon dioxide levels. Finally, geoengineering techniques of radiative forcing alter the earth’s radiative energy budget to stabilize or reduce global temperatures. It is evident that conventional mitigation efforts alone are not sufficient to meet the targets stipulated by the Paris agreement; therefore, the utilization of alternative routes appears inevitable. While various technologies presented may still be at an early stage of development, biogenic-based sequestration techniques are to a certain extent mature and can be deployed immediately.
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                Author and article information

                Journal
                JACS Au
                JACS Au
                au
                jaaucr
                JACS Au
                American Chemical Society
                2691-3704
                13 December 2023
                22 January 2024
                : 4
                : 1
                : 101-115
                Affiliations
                []Linda and Bipin Doshi Department of Chemical and Biochemical Engineering, Missouri University of Science and Technology , Rolla, Missouri 65409-1230, United States
                []National Energy Technology Laboratory, United States Department of Energy , Pittsburgh, Pennsylvania 15236, United States
                [§ ]Department of Chemical, Environmental and Materials Engineering, University of Miami , Miami, Florida 33124, United States
                Author notes
                Author information
                https://orcid.org/0000-0001-5228-5624
                https://orcid.org/0000-0002-4214-4235
                Article
                10.1021/jacsau.3c00553
                10807010
                38274256
                018129b7-3980-47de-8e22-4ff0bc6fedfe
                © 2023 The Authors. Published by American Chemical Society

                Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works ( https://creativecommons.org/licenses/by-nc-nd/4.0/).

                History
                : 18 September 2023
                : 22 November 2023
                : 19 November 2023
                Funding
                Funded by: National Science Foundation, doi 10.13039/100000001;
                Award ID: CBET-2316143
                Categories
                Article
                Custom metadata
                au3c00553
                au3c00553

                reactive capture of co2,bifunctional materials,structured monolith,methane dry reforming,hydrogen production

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