Light-facilitated structure reconstruction on self-optimized photocatalyst TiO2@BiOCl for selectively efficient conversion of CO2 to CH4

Li, Rongjie; Luan, Qingjie; Dong, Chen; Dong, Wenjun; Tang, Wenting; Wang, Ge; Lu, Yunfeng

doi:10.1016/j.apcatb.2020.119832

Cited by 107 publications

(34 citation statements)

References 60 publications

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“…[52] Cu species can also preferably enhance the adsorption and activation of the CH 3 OH* intermediate featured at 1014 cm À1 . [29,53] The formation of CH 4 is thermodynamically more feasible than the formation of CO. Thus, CH 4 can be produced via a continuous hydrogenation process at the Cu-CO complex by accepting more electrons and protons.…”

Section: Resultsmentioning

confidence: 99%

Selective CO₂‐to‐CH₄ Photoconversion in Aqueous Solutions Catalyzed by Atomically Dispersed Copper Sites Anchored on Ultrathin Graphdiyne Oxide Nanosheets

Wang

et al. 2021

Solar RRL

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Photocatalytic conversion of carbon dioxide (CO2) into chemical fuels using sunlight represents an intriguing approach to simultaneously address energy and environmental issues. However, steering the reaction pathways during the photocatalytic reduction of CO2 to selectively produce desirable hydrocarbon fuels such as methane (CH4) remains a significant challenge. Meanwhile, suppressing the hydrogen evolution reaction is extremely difficult when the photocatalytic process is carried out in aqueous solutions. Herein, ultrathin graphdiyne oxide nanosheets prepared by oxidizing and exfoliating from as‐synthesized graphdiyne are used to activate coordinated Cu2+ sites without using additional organic ligands for selective reduction of CO2 to CH4 in aqueous solutions. It is shown that the reaction selectivity toward CH4 and CO production can reach 87% and 13%, respectively, whereas the hydrogen evolution reaction can be completely inhibited. The atomically anchored Cu2+ ions can effectively trap photogenerated electrons and serve as active sites for the selective CO2‐to‐CH4 conversion. Considering the rich coordination chemistry of polymer materials, the methodology presented in this study can be extended to prepare various polymer‐based photocatalysts with precisely engineered metallic centers toward the selective reduction of CO2 to chemical fuels.

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Section: Resultsmentioning

confidence: 99%

Selective CO₂‐to‐CH₄ Photoconversion in Aqueous Solutions Catalyzed by Atomically Dispersed Copper Sites Anchored on Ultrathin Graphdiyne Oxide Nanosheets

Wang

et al. 2021

Solar RRL

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“…The synergies between OV-rich TiO 2 and other cocatalysts have been extensively explored in recent years. Li et al [102] reported a TiO 2 @BiOCl (TBC) photocatalyst which achieved the highest CH 4 productivity rate of 168.5 µmol g −1 h −1 and optimal CH 4 selectivity of 99.4%, a remarkable photocatalysis performance in CO 2 reduction. The H-incorporated vacancy is formed by modification of H on the OV, which remarkably weakens H 2 O adsorption capacity and hinders H 2 generation.…”

Section: Vacancies and Other Defectsmentioning

confidence: 99%

Emerging Strategies for CO₂ Photoreduction to CH₄: From Experimental to Data‐Driven Design

Cheng

Sun

Lim

et al. 2022

Advanced Energy Materials

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been described as a key metric for understanding the effects of global warming due to its direct impact on climate change. [2] Extensive modeling with energy-economyenvironment scenarios or projections to keep the global temperature from rising above 1.5 °C by the year 2100 shows that such a positive outlook is only possible if the global energy system is completely decarbonized (i.e., net-zero global CO 2 emissions) by mid-century, followed by active CO 2 removal (i.e., carbon-negative) in the second half of the century. [3] The catalytic conversion of CO 2 to valuable energy-related products (e.g., syngas, CH 4 , CH 3 OH, and longer-chain hydrocarbons) [4] by thermal reforming and hydrogenation, [5][6][7][8][9][10][11] electrocatalysis, [12][13][14] or photocatalysis [15] could occupy an important position in a future carbon-negative economy by directly replacing nonrenewable sources of these molecules, provided that the energy inputs to these processes are themselves derived from renewable sources. [16,17] In this regard, photocatalytic strategies stand out by not requiring a secondary medium of energy storage, and being able to realize the CO 2 conversion into high value-added fuels directly via renewable solar energy without external energy input. [18] Indeed, photocatalytic CO 2 reduction has been considered to be a "kill two birds with one stone" approach for sustainable energy production and greenhouse gas reduction. [19] In contrast, thermocatalytic approachesThe solar-energy-driven photoreduction of CO 2 has recently emerged as a promising approach to directly transform CO 2 into valuable energy sources under mild conditions. As a clean-burning fuel and drop-in replacement for natural gas, CH 4 is an ideal product of CO 2 photoreduction, but the development of highly active and selective semiconductor-based photocatalysts for this important transformation remains challenging. Hence, significant efforts have been made in the search for active, selective, stable, and sustainable photocatalysts. In this review, recent applications of cutting-edge experimental and computational materials design strategies toward the discovery of novel catalysts for CO 2 photocatalytic conversion to CH 4 are systematically summarized. First, insights into effective experimental catalyst engineering strategies, including heterojunctions, defect engineering, cocatalysts, surface modification, facet engineering, and single atoms, are presented. Then, datadriven photocatalyst design spanning density functional theory (DFT) simulations, high-throughput computational screening, and machine learning (ML) is presented through a step-by-step introduction. The combination of DFT, ML, and experiments is emphasized as a powerful solution for accelerating the discovery of novel catalysts for photocatalytic reduction of CO 2 . Last, challenges and perspectives concerning the interplay between experiments and data-driven rational design strategies for the industrialization of large-scale CO 2 photoreduction technologies are described.

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“…In addition, a self-optimized TiO 2 @BiOCl photocatalyst can gather electrons efficiently to accelerate the photocatalytic efficiency and selectively efficiently convert CO 2 to CH 4 , which was prepared by facile growth of ultrathin BiOCl lamina on the defective surfaces of TiO 2 nanotubes. 51 However, the process of TiO 2 transformation from a rigid crystal structure into a spatially anisotropic helical structure remains a challenge. In 2002, TiO 2 helical nanoribbons were assembled by helical organogels as templates.…”

Section: Introductionmentioning

confidence: 99%

“…The annealed SiO x –TiO 2 nanowires enhance the optical absorption with an improved crystal structure and elimination of the interface trap states to further improve the light detection ability. In addition, a self-optimized TiO 2 @BiOCl photocatalyst can gather electrons efficiently to accelerate the photocatalytic efficiency and selectively efficiently convert CO 2 to CH 4 , which was prepared by facile growth of ultrathin BiOCl lamina on the defective surfaces of TiO 2 nanotubes . However, the process of TiO 2 transformation from a rigid crystal structure into a spatially anisotropic helical structure remains a challenge.…”

Section: Introductionmentioning

confidence: 99%

Fabrication and Elastic Properties of TiO₂ Nanohelix Arrays through a Pressure-Induced Hydrothermal Method

et al. 2021

Self Cite

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TiO 2 nanohelices (NHs) have attracted extensive attention owing to their high aspect ratio, excellent flexibility, elasticity, and optical properties, which endow promising performances in a vast range of vital fields, such as optics, electronics, and micro/nanodevices. However, preparing rigid TiO 2 nanowires (TiO 2 NWs) into spatially anisotropic helical structures remains a challenge. Here, a pressure-induced hydrothermal strategy was designed to assemble individual TiO 2 NWs into a DNA-like helical structure, in which a Teflon block was placed in an autoclave liner to regulate system pressure and simulate a cell-rich environment. The synthesized TiO 2 NHs of 50 nm in diameter and 5−7 mm in length approximately were intertwined into nanohelix bundles (TiO 2 NHBs) with a diameter of 20 μm and then assembled into vertical TiO 2 nanohelix arrays (NHAs). Theoretical calculations further confirmed that straight TiO 2 NWs prefer to convert into helical conformations with minimal entropy (S) and free energy (F) for continuous growth in a confined space. The excellent elastic properties exhibit great potential for applications in flexible devices or buffer materials.

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Light-facilitated structure reconstruction on self-optimized photocatalyst TiO2@BiOCl for selectively efficient conversion of CO2 to CH4

Cited by 107 publications

References 60 publications

Selective CO₂‐to‐CH₄ Photoconversion in Aqueous Solutions Catalyzed by Atomically Dispersed Copper Sites Anchored on Ultrathin Graphdiyne Oxide Nanosheets

Selective CO₂‐to‐CH₄ Photoconversion in Aqueous Solutions Catalyzed by Atomically Dispersed Copper Sites Anchored on Ultrathin Graphdiyne Oxide Nanosheets

Emerging Strategies for CO₂ Photoreduction to CH₄: From Experimental to Data‐Driven Design

Fabrication and Elastic Properties of TiO₂ Nanohelix Arrays through a Pressure-Induced Hydrothermal Method

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Light-facilitated structure reconstruction on self-optimized photocatalyst TiO2@BiOCl for selectively efficient conversion of CO2 to CH4

Cited by 107 publications

References 60 publications

Selective CO2‐to‐CH4 Photoconversion in Aqueous Solutions Catalyzed by Atomically Dispersed Copper Sites Anchored on Ultrathin Graphdiyne Oxide Nanosheets

Selective CO2‐to‐CH4 Photoconversion in Aqueous Solutions Catalyzed by Atomically Dispersed Copper Sites Anchored on Ultrathin Graphdiyne Oxide Nanosheets

Emerging Strategies for CO2 Photoreduction to CH4: From Experimental to Data‐Driven Design

Fabrication and Elastic Properties of TiO2 Nanohelix Arrays through a Pressure-Induced Hydrothermal Method

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Selective CO₂‐to‐CH₄ Photoconversion in Aqueous Solutions Catalyzed by Atomically Dispersed Copper Sites Anchored on Ultrathin Graphdiyne Oxide Nanosheets

Selective CO₂‐to‐CH₄ Photoconversion in Aqueous Solutions Catalyzed by Atomically Dispersed Copper Sites Anchored on Ultrathin Graphdiyne Oxide Nanosheets

Emerging Strategies for CO₂ Photoreduction to CH₄: From Experimental to Data‐Driven Design

Fabrication and Elastic Properties of TiO₂ Nanohelix Arrays through a Pressure-Induced Hydrothermal Method