Solar‐driven synthesis of hydrogen peroxide (H2O2) through photocatalysis stands out as a promising avenue for sustainable energy generation, marked by environmental friendliness and industrial feasibility. However, the inherent limitations of carbon nitride (CN) in photocatalytic H2O2 production significantly impede their performance. Herein, a novel 0D/2D carbon dots‐modified CN nanosheet heterojunction (CDsMCN) is introduced, synthesized through a hydrothermal‐calcination tandem strategy induced by CDs derived from melamine. This innovative technique enhances the n→π* electronic transition in CDsMCN, accelerating the separation efficiency of electron‐hole pairs, boosting oxygen adsorption, and promoting a highly selective 2e− ORR. Comparative to pristine CN, CDs10MCN exhibited a remarkable tenfold increase in H2O2 production, reaching an impressive 1.48 mmol L−1. Furthermore, CDs10MCN demonstrates exceptional stability, maintaining its catalytic efficiency at the initial level over four consecutive cycles. The notable achievement of a molar selectivity of H2O2 ≈80% at an onset potential of 0.6 V (vs RHE) underscores its exceptional ability to produce the desired product selectively. Advanced in situ characterization together with DFT calculations revealed that the ultrathin CDs10MCN nanosheet heterojunction with enhanced n→π* electronic transition improves its optical properties, reduces bandgap, facilitates fast charge migration, and increases photocatalytic H2O2 performance, thereby serving as a promising candidate for advanced catalytic applications.

Nitrogen‐Rich Carbon Dot‐Mediated n→π* Electronic Transition in Carbon Nitride for Superior Photocatalytic Hydrogen Peroxide Production

For over a century, enzyme immobilisation has been proven to be a superior strategy to improve catalytic activity and reusability and ensure easy separation, easy operation, and reduced cost. Enzyme immobilisation allows for an easier separation of the enzyme from the reaction mixture, thus simplifying downstream processing. This technology protects the enzyme from degradation or inactivation by harsh reaction conditions, making it more robust and suitable to be used in various applications. Recent strategies of immobilisation methods, such as adsorption, cross-linking, entrapment or encapsulation, and covalent bonding, were critically reviewed. These strategies have shown promising results in improving enzyme stability, activity, and reusability in various applications. A recent development in enzyme immobilisation in nanomaterials and agrowaste renewable carriers is underlined in the current review. Furthermore, the use of nanomaterials and agrowaste carriers in enzyme immobilisation has gained significant attention due to their unique properties, such as high surface area, high mass transfer, biocompatibility, and sustainability. These materials offer promising outcomes for developing more efficient and sustainable immobilised enzymes. This state-of-the-art strategy allows for better control over enzyme reactions and enhances their reusability, leading to more cost-effective and environmentally friendly processes. The use of renewable materials also helps to reduce waste generation and promote the utilisation of renewable resources, further contributing to the development of a circular economy. 

Recent Advances in Enzyme Immobilisation Strategies: An Overview of Techniques and Composite Carriers

Engineering the specific active sites of photocatalysts for simultaneously promoting CO2 and H2O activation is important to achieve the efficient conversion of CO2 to hydrocarbon with H2O as a proton source under sunlight. Herein, we delicately design the In/TiO2-VO photocatalyst by engineering In single atoms (SAs) and oxygen vacancies (VOs) on porous TiO2. The relation between structure and performance of the photocatalyst is clarified by both experimental and theoretical analyses at the atomic levels. The In/TiO2-VO photocatalyst furnish a high CH4 production rate up to 35.49 μmol g−1 h−1 with a high selectivity of 91.3% under simulated sunlight, while only CO is sluggishly generated on TiO2-VO. The combination of in situ spectroscopic analyses with theoretical calculations reveal that the VO sites accelerate H2O dissociation and increase proton feeding for CO2 reduction. Furthermore, the VO regulated In-Ti dual sites enable the formation of a stable adsorption conformation of In-C-O-Ti intermediate, which is responsible for the highly selective reduction of CO2 to CH4. This work demonstrates a new strategy for the development of effective photocatalysts by coupling metal SA sites with the adjacent metal sites of support to synergistically enhance the activity and selectivity of CO2 photoreduction. 

Promoting CO2 and H2O activation on O-vacancy regulated In-Ti dual-sites for enhanced CH4 photo-production

Imitating catalytic sites of natural enzymes is a promising approach to accurately improve the catalytic performances of nanozymes. Herein, inspired by the structure of natural horseradish peroxidase (HRP), three-component condensation strategy is unitized to design histidine (His) functionalized iron porphyrin covalent organic frameworks (Fe-COF-H3) nanozyme with peroxidase-like (POD-like) activity. The introduced His could form favorable microenvironment around the iron porphyrin structure, enhancing the catalytic capacity of COF nanozyme. Taking advantage of its excellent POD-like activity, Fe-COF-H3 was utilized as a carrier to immobilize urate oxidase (UOx) for the construction of enzyme-nanozyme cascade system (UOx@Fe-COF-H3). The UOx@Fe-COF-H3 was successfully applied for the colorimetric detection of uric acid (UA) in biological samples. This work not only offers a new insight to develop high-efficiency COF nanozymes, but also expands the application of COF nanozyme for the construction of enzyme-nanozyme cascade system. 

Bioinspired construction of histidine-doped porphyrin covalent organic framework nanozyme with enhanced peroxidase-like activity for sensitive uric acid detection

A novel approach for the enzymatic esterification of carbohydrate polyols with fatty acids was investigated, with reactive natural deep eutectic solvents (R-NADES) as reaction medium and source of reagents. Three binary hydrophilic R-NADES consisting of choline chloride (ChCl) as hydrogen bond acceptor (HBA) and sugar alcohols (D-sorbitol, xylitol, D-arabitol) as hydrogen bond donors (HBD), were prepared and characterized. The carbohydrate polyol-based R-NADES were durable viscous fluids between 40 and 80⁰C, the common temperature range for an enzymatic reaction. The commercially accessible lipase B from Candida antarctica immobilized on acrylic resins (LAR) showed significant esterification activity and exceptional thermal stability in all three tested R-NADES and successfully catalyzed the synthesis of polyol esters. Box Behnken factorial design with three levels-three variables was used for optimizing the reaction conditions. The preparative esterification of D-arabitol with lauric acid (LA) at predicted optimal values for enzyme load, (i.e., 800 U/gram D-arabitol), temperature (70 °C) and LA/D-arabitol molar ratio of 1), attained 80 mol% LA conversion after 24 h reaction time. Structural analysis based on mass, infrared and nuclear magnetic resonance spectroscopy demonstrated that the reaction product is solely the diester 1,5-dilauryl-D-arabitol (1,5-DLDA). The 1,5-DLDA product, with an NMR-purity above 99.9%, was isolated in 95% yield. Under similar conditions, 1,5-dilauryl-xylitol (1,5-DLX) and 1,6-dilauryl-D-sorbitol (1,6-DLDS) were obtained, at a LA conversion of 56 mol% and 62 mol%, respectively. A combination of docking and molecular dynamics simulations allowed to rationalize the structural stability of the lipase B from Candida antarctica (CalB) active site in R-NADES, as well as the selectivity of the catalyzed esterification. 

Reactive natural deep eutectic solvents increase selectivity and efficiency of lipase catalyzed esterification of carbohydrate polyols

Unspecific peroxygenases immobilized on Pd-loaded three-dimensional ordered macroporous (3DOM) titania photocatalyst for photo-enzyme integrated catalysis

A three-in-one heterogeneous catalyst (UPO@dTiO2-CD) was fabricated by grafting cyclodextrins (CDs) on the dehiscent TiO2 (dTiO2) surface and subsequently immobilizing unspecific peroxygenase (rAaeUPO), which exhibited double enhanced electron/mass transfer in photo-enzymatic enantioselective hydroxylation of the C-H bond. The tunable anatase/rutile phase ratio and dehiscent mesoporous architectures of dTiO2 and the electron donor feature and hydrophobic inner cavity of the CDs are independently responsible for accelerating both electron and mass transfer. The coordination of the photocatalytic and enzymatic steps was achieved by structural and compositional regulation. The optimized UPO@dTiO2-CD not only displayed high catalytic efficiency (turnover number and turnover frequency of rAaeUPO up to >65,000 and 91 min-1, respectively) but also exhibited high stability and reusability.

Immobilization of Enzymes on Cyclodextrin-Anchored Dehiscent Mesoporous TiO2 for Efficient Photoenzymatic Hydroxylation.

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Unspecific peroxygenases immobilized on Pd-loaded three-dimensional ordered macroporous (3DOM) titania photocatalyst for photo-enzyme integrated catalysis

Immobilization of Enzymes on Cyclodextrin-Anchored Dehiscent Mesoporous TiO2 for Efficient Photoenzymatic Hydroxylation.