Abstract:Photocatalytic reforming of lignocellulosic biomass is an emerging approach to produce renewable H
2
. This process combines photo‐oxidation of aqueous biomass with photocatalytic hydrogen evolution at ambient temperature and pressure. Biomass conversion is less energy demanding than water splitting and generates high‐purity H
2
without O
2
production. Direct photoreforming of raw, unprocessed biomass has the potential to provide affordable a… Show more
“…[1] Light-driven water splitting into hydrogen is av ery active field of energy research for the most promising strategies to obtain alternative energy sources. [3] Covalent organic frameworks (COFs) and metalorganic frameworks (MOFs), as crystalline and porous materials assembled with pure organic molecules or and metal ions (metal clusters) by covalent or coordinated bonds, have been employed for various areas such as gas storage, [4] catalysis, [5] and sensing. [3] Covalent organic frameworks (COFs) and metalorganic frameworks (MOFs), as crystalline and porous materials assembled with pure organic molecules or and metal ions (metal clusters) by covalent or coordinated bonds, have been employed for various areas such as gas storage, [4] catalysis, [5] and sensing.…”
Crystalline and porous covalent organic frameworks (COFs) and metal-organic frameworks (MOFs) materials have attracted enormous attention in the field of photocatalytic H evolution due to their long-range order structures, large surface areas, outstanding visible light absorbance, and tunable band gaps. In this work, we successfully integrated two-dimensional (2D) COF with stable MOF. By covalently anchoring NH -UiO-66 onto the surface of TpPa-1-COF, a new type of MOF/COF hybrid materials with high surface area, porous framework, and high crystallinity was synthesized. The resulting hierarchical porous hybrid materials show efficient photocatalytic H evolution under visible light irradiation. Especially, NH -UiO-66/TpPa-1-COF (4:6) exhibits the maximum photocatalytic H evolution rate of 23.41 mmol g h (with the TOF of 402.36 h ), which is approximately 20 times higher than that of the parent TpPa-1-COF and the best performance photocatalyst for H evolution among various MOF- and COF-based photocatalysts.
“…[1] Light-driven water splitting into hydrogen is av ery active field of energy research for the most promising strategies to obtain alternative energy sources. [3] Covalent organic frameworks (COFs) and metalorganic frameworks (MOFs), as crystalline and porous materials assembled with pure organic molecules or and metal ions (metal clusters) by covalent or coordinated bonds, have been employed for various areas such as gas storage, [4] catalysis, [5] and sensing. [3] Covalent organic frameworks (COFs) and metalorganic frameworks (MOFs), as crystalline and porous materials assembled with pure organic molecules or and metal ions (metal clusters) by covalent or coordinated bonds, have been employed for various areas such as gas storage, [4] catalysis, [5] and sensing.…”
Crystalline and porous covalent organic frameworks (COFs) and metal-organic frameworks (MOFs) materials have attracted enormous attention in the field of photocatalytic H evolution due to their long-range order structures, large surface areas, outstanding visible light absorbance, and tunable band gaps. In this work, we successfully integrated two-dimensional (2D) COF with stable MOF. By covalently anchoring NH -UiO-66 onto the surface of TpPa-1-COF, a new type of MOF/COF hybrid materials with high surface area, porous framework, and high crystallinity was synthesized. The resulting hierarchical porous hybrid materials show efficient photocatalytic H evolution under visible light irradiation. Especially, NH -UiO-66/TpPa-1-COF (4:6) exhibits the maximum photocatalytic H evolution rate of 23.41 mmol g h (with the TOF of 402.36 h ), which is approximately 20 times higher than that of the parent TpPa-1-COF and the best performance photocatalyst for H evolution among various MOF- and COF-based photocatalysts.
“…[1] Alternatively,t his reactionc an be undertaken through the oxidation of organic species, either in the form of biomass-derived substrates,s uch as EtOH, MeOH,g lucoseo rl ignocellulose, [2][3][4] or throughs elective organic oxidation reactions to generate higher-value products. These systemsa re typicallyl imited to anaerobic conditions due to the inhibiting effects of O 2 .H ere, we report that sacrificialH 2 evolution with CdS quantum dots does not necessarily suffer from O 2 inhibition and can even be stabilised under aerobic conditions.…”
mentioning
confidence: 99%
“…[1] Alternatively,t his reactionc an be undertaken through the oxidation of organic species, either in the form of biomass-derived substrates,s uch as EtOH, MeOH,g lucoseo rl ignocellulose, [2][3][4] or throughs elective organic oxidation reactions to generate higher-value products. [1] Alternatively,t his reactionc an be undertaken through the oxidation of organic species, either in the form of biomass-derived substrates,s uch as EtOH, MeOH,g lucoseo rl ignocellulose, [2][3][4] or throughs elective organic oxidation reactions to generate higher-value products.…”
Photocatalytic H production through water splitting represents an attractive route to generate a renewable fuel. These systems are typically limited to anaerobic conditions due to the inhibiting effects of O . Here, we report that sacrificial H evolution with CdS quantum dots does not necessarily suffer from O inhibition and can even be stabilised under aerobic conditions. The introduction of O prevents a key inactivation pathway of CdS (over-accumulation of metallic Cd and particle agglomeration) and thereby affords particles with higher stability. These findings represent a possibility to exploit the O reduction reaction to inhibit deactivation, rather than catalysis, offering a strategy to stabilise photocatalysts that suffer from similar degradation reactions.
“… Erwin Reisner (University of Cambridge) was featured here when he joined the Editorial Board of Angewandte Chemie . His recent contributions to the journal include a Minireview on solar hydrogen generation from lignocellulose …”
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