Artificial photosynthesis (Washington, D.C.)最新文献

Photophysics of Doubly Reduced Quinacridone Dyes: Toward Redox Reactivity Activated by Red Light. 双还原喹吖酮染料的光物理：红光活化的氧化还原反应性。

Artificial photosynthesis (Washington, D.C.) Pub Date : 2026-05-18 eCollection Date: 2026-09-24 DOI: 10.1021/aps.6c00006

Elena Rossin, Björn Pfund, Martina Chirico, Tobia Casadei, Giacomo Morselli, Catia Nicoletti, Mathis Brändlin, Sara Bonacchi, Marco Fantin, Pierluca Galloni, Oliver S Wenger, Andrea Sartorel

{"title":"Photophysics of Doubly Reduced Quinacridone Dyes: Toward Redox Reactivity Activated by Red Light.","authors":"Elena Rossin, Björn Pfund, Martina Chirico, Tobia Casadei, Giacomo Morselli, Catia Nicoletti, Mathis Brändlin, Sara Bonacchi, Marco Fantin, Pierluca Galloni, Oliver S Wenger, Andrea Sartorel","doi":"10.1021/aps.6c00006","DOIUrl":"10.1021/aps.6c00006","url":null,"abstract":"Super-reductive photocatalysis is an emerging approach to broaden the conventional organic reactivity by exploiting reduced forms of a parent photocatalyst (PC) as the actual photoactive super-reductant. Recent reports have highlighted the advantages of using closed-shell, doubly reduced PC2- with respect to open-shell, singly reduced PC•-, with the former having longer excited-state lifetime and enlarged reductive power. It is thus important to expand the families of super-reductants that fit these features. In this work, we investigate doubly reduced N,N-dialkylated derivatives of quinacridone (QA) industrial pigment as potential super-reductants, exploiting the use of low-energy red light. These give the possibility of electrochemically generating the radical anion and dianion forms, with the latter being characterized by an emissive excited state with nanosecond lifetimes (compared to ps lifetime of the radical anion excited state) and reductive power up to -3.5 V vs Saturated Calomel Electrode, ca. 0.9 V enhanced with respect to the radical anion excited state. The super-reductant activity of the bis-reduced species is demonstrated in the challenging reductive deamination of arylammonium derivatives. All-in-one, these findings will inspire the design of closed-shell super-redox photocatalysts based on industrial pigments, thus impacting sectors involving organic reactivity, photocatalysis, and sustainable chemistry.","PeriodicalId":520501,"journal":{"name":"Artificial photosynthesis (Washington, D.C.)","volume":"2 5","pages":"263-272"},"PeriodicalIF":0.0,"publicationDate":"2026-05-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13618248/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149077336","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Reducing Flavin and Ubiquinone Headgroups with Silicon Nanowire Photocathodes. 用硅纳米线光电阴极还原黄素和泛醌头基团。

Artificial photosynthesis (Washington, D.C.) Pub Date : 2026-03-30 eCollection Date: 2026-07-23 DOI: 10.1021/aps.6c00003

Elizabeth Lineberry, Andrew Liu, Nathan E Soland, Wonseok Lee, Lihini Jayasinghe, Peidong Yang

{"title":"Reducing Flavin and Ubiquinone Headgroups with Silicon Nanowire Photocathodes.","authors":"Elizabeth Lineberry, Andrew Liu, Nathan E Soland, Wonseok Lee, Lihini Jayasinghe, Peidong Yang","doi":"10.1021/aps.6c00003","DOIUrl":"10.1021/aps.6c00003","url":null,"abstract":"Photosynthetic biohybridsa structure composed of semiconducting electrodes and carbon dioxide-fixing autotrophs which can be energized by the electrodeoffer a promising platform for selective CO2 reduction. However, studying the charge-transfer mechanisms from the semiconductor to the cell proves challenging due to a variety of simultaneous processes. Therefore, to deconvolute the system to understand photoelectrochemical performance, we employ model systems composed of a subset of the electron-transfer pathway. Here, we photoelectrochemically reduced ubiquinone-0 (UQ0) and riboflavin (Rf) (the head groups of ubiquinone-8/10 and flavin mononucleotide/flavin adenine dinucleotide) using Pt-decorated n+p-silicon nanowires, a robust catalytic architecture. Under irradiation with 100 mW cm-2 red light (740 nm), UQ0 and Rf were reduced with onset potentials of 0.876 V vs the reversible hydrogen electrode (VRHE) and 0.691 VRHE, respectively. In addition, UQ0 achieved a maximum Faradaic efficiency (FE) of 81% with a conversion rate of 1.22 μmol cm-2 h-1 at 0.75 VRHE, while Rf reached its maximum FE and rate at 73% and 0.167 μmol cm-2 h-1, respectively, at 0.55 VRHE. Both redox cofactors were continuously reduced over a 12 h period, demonstrating the robust photosynthetic biohybrid system.","PeriodicalId":520501,"journal":{"name":"Artificial photosynthesis (Washington, D.C.)","volume":"2 4","pages":"234-242"},"PeriodicalIF":0.0,"publicationDate":"2026-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13403228/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148612154","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A Multifaceted Vision of Challenges and Opportunities in Practical Artificial Photosynthesis Devices. 实用人工光合作用装置的挑战与机遇。

Artificial photosynthesis (Washington, D.C.) Pub Date : 2026-01-29 eCollection Date: 2026-03-26 DOI: 10.1021/aps.5c00034

Siglinda Perathoner, Can Li, Jijie Wang, Rengui Li, Wangyin Wang, Gabriele Centi, Valentino Romano

引用次数: 0

Efficient and Robust Hybrid Molecular Photoanodes for Water Oxidation at Neutral pH Based on Ru Complexes Covalently Bonded to Polymeric Carbon Nitride. 基于Ru络合物共价键合聚合氮化碳的中性pH水氧化高效、坚固的杂化分子光阳极。

Artificial photosynthesis (Washington, D.C.) Pub Date : 2025-09-16 eCollection Date: 2026-01-22 DOI: 10.1021/aps.5c00019

Martina Salati, Sanjit Mondal, Michael Volokh, Josep Albero, Hermenegildo García, Marcos Gil-Sepulcre, Menny Shalom, Antoni Llobet

{"title":"Efficient and Robust Hybrid Molecular Photoanodes for Water Oxidation at Neutral pH Based on Ru Complexes Covalently Bonded to Polymeric Carbon Nitride.","authors":"Martina Salati, Sanjit Mondal, Michael Volokh, Josep Albero, Hermenegildo García, Marcos Gil-Sepulcre, Menny Shalom, Antoni Llobet","doi":"10.1021/aps.5c00019","DOIUrl":"10.1021/aps.5c00019","url":null,"abstract":"Light-induced water splitting (hν-WS) represents a promising strategy for the sustainable generation of green hydrogen. In particular, the photoelectrochemical water oxidation (WO) reaction remains a critical step due to its kinetic and thermodynamic demands. Heterostructures comprising water oxidation catalysts (WOCs) integrated with photoactive materials, such as polymeric carbon nitride (CN), have demonstrated potential for enhancing the performance owing to their favorable energetics, cost-effectiveness, and device simplicity. However, intrinsic limitations of CN, including poor charge separation and electron transfer properties, limited activity, and stability under near-neutral conditions, hinder its practical application. To address these challenges, we report the covalent functionalization of CN with a Ru-based molecular WOC, yielding hybrid photoelectrode CN TM @Ru. The photoelectrocatalytic activity of CN TM @Ru toward WO was evaluated under simulated solar irradiation (1 sun), displaying a sustained photocurrent density of ∼480 μA cm-2 at 1.23 V vs RHE over 15 h (TON > 2000) at neutral pH. Comprehensive photophysical analyses revealed enhanced charge separation and interfacial charge-transfer dynamics, corroborating the synergistic role of the covalently anchored molecular catalyst in facilitating multielectron transfer steps and enabling efficient water oxidation catalysis.","PeriodicalId":520501,"journal":{"name":"Artificial photosynthesis (Washington, D.C.)","volume":"2 1","pages":"43-52"},"PeriodicalIF":0.0,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12833802/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146069502","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Axiomatic Design for Analysis and Noniterative Engineering of Photoelectrochemical Cells for CO₂ Conversion at High Photon to Product Yield. 高光子产率CO2转化的光电化学电池的分析和非迭代工程的公理化设计。

Artificial photosynthesis (Washington, D.C.) Pub Date : 2025-06-17 eCollection Date: 2025-09-25 DOI: 10.1021/aps.5c00004

Suzanne M E Assen, G J Agur Sevink, Huub J M de Groot

{"title":"Axiomatic Design for Analysis and Noniterative Engineering of Photoelectrochemical Cells for CO2 Conversion at High Photon to Product Yield.","authors":"Suzanne M E Assen, G J Agur Sevink, Huub J M de Groot","doi":"10.1021/aps.5c00004","DOIUrl":"10.1021/aps.5c00004","url":null,"abstract":"An Axiomatic Design (AD) theoretical protocol is proposed for the analysis and noniterative engineering of photoelectrochemical (PEC) cells that can convert CO2 toward C2+ products. AD provides criteria for identifying and selecting materials based on data commonly available in the literature. In addition, it establishes a design order for how to achieve optimal integration of materials for catalysis and light-induced charge separation with a proton-transporting membrane in a noniterative manner by matching relevant fluxes with concentration at interfaces across the design. For a hypothetical tandem PEC flow cell reactor for ethylene as an example, the AD protocol predicts an upper bound of 31 μmol h-1 cm-2 at 12% solar-to-product efficiency following PEC process optimization with a design path comprising five steps, starting from data for an O-(II)-D-Cu CO2 reduction reaction (CO2RR) catalyst and including current concentration to tailor the overpotential. The computational procedure provides models with high yield and robustness by balancing high selectivity with low overpotential and a broad operation range of 0.5-1.2 Sun with a dual absorber with bandgaps of 1.90 and 1.35 eV and a fill factor of 0.85. The procedures are implemented in Python and use a decoupled design matrix that eliminates interdependencies between components.","PeriodicalId":520501,"journal":{"name":"Artificial photosynthesis (Washington, D.C.)","volume":"1 5","pages":"237-250"},"PeriodicalIF":0.0,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12481723/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145208882","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Oxygen-Mediated Sequential Down-Conversion in Perylenediimides. 氧介导的苝酰二亚胺的序贯降转化。

Artificial photosynthesis (Washington, D.C.) Pub Date : 2025-06-01 eCollection Date: 2025-09-25 DOI: 10.1021/aps.5c00002

Yifan Bo, Nathalie Zink-Lorre, René Weiß, Ángela Sastre-Santos, Timothy Clark, Fernando Fernández-Lázaro, Dirk M Guldi

{"title":"Oxygen-Mediated Sequential Down-Conversion in Perylenediimides.","authors":"Yifan Bo, Nathalie Zink-Lorre, René Weiß, Ángela Sastre-Santos, Timothy Clark, Fernando Fernández-Lázaro, Dirk M Guldi","doi":"10.1021/aps.5c00002","DOIUrl":"10.1021/aps.5c00002","url":null,"abstract":"Perylenediimides (PDIs) are among the best-known chromophores for optoelectronic applications. Their photophysics in oxygen-rich environments remains, however, underexplored. In this study, we investigate three different PDI derivatives using steady-state and time-resolved absorption and emission spectroscopy in toluene with different oxygen concentrations. Unsubstituted PDI and 1,7-bay-substituted PDI featuring diphenylphenoxy groups exhibit oxygen-mediated sequential down-conversion. Upon photoexcitation, the singlet excited state (S1) of PDIs interacts with molecular oxygen (3O2) to generate singlet oxygen (1O2) via the formation of the triplet excited state (T1) of PDIs. Subsequently, (T1)-s of PDIs sensitize an additional 3O2 to produce a second 1O2. Overall, one (S1) produces two 1O2. Importantly, this process depends on energy requirements: on one hand, the energy difference between (S1) and (T1), and on the other hand, the (T1) energy level should exceed that of 1O2. Our work illustrates the oxygen-mediated sequential down-conversion in perylenediimides and reveals its effects.","PeriodicalId":520501,"journal":{"name":"Artificial photosynthesis (Washington, D.C.)","volume":"1 5","pages":"226-236"},"PeriodicalIF":0.0,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12481719/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145208896","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Unidirectional Transmembrane Photoinduced Electron Transfer with Artificial Metallopeptides. 人工金属肽单向跨膜光诱导电子转移。

Artificial photosynthesis (Washington, D.C.) Pub Date : 2025-05-28 eCollection Date: 2025-07-24 DOI: 10.1021/aps.5c00010

David M Klein, Xinmeng Li, Aimee L Boyle, Rianne van der Pol, Vasiliki E Tsina, G J Agur Sevink, Albert M Brouwer, Sylvestre Bonnet

{"title":"Unidirectional Transmembrane Photoinduced Electron Transfer with Artificial Metallopeptides.","authors":"David M Klein, Xinmeng Li, Aimee L Boyle, Rianne van der Pol, Vasiliki E Tsina, G J Agur Sevink, Albert M Brouwer, Sylvestre Bonnet","doi":"10.1021/aps.5c00010","DOIUrl":"10.1021/aps.5c00010","url":null,"abstract":"The ability to drive unidirectional photoinduced electron transfer through an insulating lipid membrane is one of the most striking features of the thylakoid membrane, and recreating this property artificially is considered as one of the holy grails of artificial photosynthesis. Here, we report two artificial metallopeptides, WALP23-Re 2 and WALP23-Ru 2 , that were embedded in the membrane of dissymmetric liposomes containing an electron donor in the inner compartment and an electron acceptor in the bulk aqueous phase. Upon light irradiation under air, unidirectional electron transfer was observed from one side of the membrane to the other one with both metallopeptides. However, the mechanism of photoinduced electron transfer strongly depended on the metal center: the neutral WALP23-Re 2 peptide achieved genuine electron transfer through the membrane, but with the tetracationic WALP23-Ru 2 peptide the transmembrane electron transfer appeared to be the result of light-induced leakage of the electron donor molecules through the lipid bilayer, followed by electron transfer on the same side of the membrane by peptides assembled parallel to the membrane. These results highlight both the unique potential of the neutral metallopeptide WALP23-Re2 to drive transmembrane photoinduced electron transfer in artificial photosynthetic systems, as well as the importance of membrane-leakage studies to validate the working mechanism of such supramolecular systems.","PeriodicalId":520501,"journal":{"name":"Artificial photosynthesis (Washington, D.C.)","volume":"1 4","pages":"188-203"},"PeriodicalIF":0.0,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12302060/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144746692","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Demonstration of the Radical Coupling Pathway in a Fast Fe-Based Water Oxidation Catalyst. 快速铁基水氧化催化剂中自由基耦合途径的论证。

Artificial photosynthesis (Washington, D.C.) Pub Date : 2025-03-03 eCollection Date: 2025-07-24 DOI: 10.1021/aps.4c00024

Jully Patel, Gabriel Bury, Roman Ezhov, Yulia Pushkar

{"title":"Demonstration of the Radical Coupling Pathway in a Fast Fe-Based Water Oxidation Catalyst.","authors":"Jully Patel, Gabriel Bury, Roman Ezhov, Yulia Pushkar","doi":"10.1021/aps.4c00024","DOIUrl":"10.1021/aps.4c00024","url":null,"abstract":"Optimization of water oxidation reaction (WOR) catalysts is critical for the development of clean energy technology based on the concept of artificial photosynthesis. Deep mechanistic insights at the molecular and electronic levels are required. Theoretically, the radical coupling (RC) mechanism should allow for a virtually barrier-less process of O-O bond formation in the WOR. This mechanism has been proposed for a number of multinuclear Fe-based water oxidation catalysts (WOCs), but its firm experimental confirmation for Fe systems is lacking. Here, we describe a RC mechanism in [(MeOH)-Fe-(Hbbpya)-μ-O-(Hbbpya)-Fe-(MeOH)]-(OTf)4 (1) (Hbbpya = N,N-bis-(2,2'-bipyrid-6-yl)-amine) and its methylated analog [(MeOH)-Fe-(CH3bbpya)-μ-O-(CH3bbpya)-Fe-(MeOH)]-(OTf)4 (1-CH 3 ). In situ XAS revealed that 1 (dimer species) breaks into monomers under catalytic conditions. The kinetic analysis has shown a second-order reaction in the catalyst, and the kinetic isotope effect has shown a minimal k H/k D ≈ 1 effect consistent with the RC pathway; EPR and XAS detected an FeVO intermediate. DFT confirmed the preference for the RC pathway. This Fe-based WOC shows a high rate of O2 evolution in chemical and photochemical WOR, comparable with some well-known Ru-based systems. These results highlight the direction for designing Fe-based WOCs with high activity and the future engineering of WOCs with the RC mechanism for functional and scalable applications for artificial photosynthesis.","PeriodicalId":520501,"journal":{"name":"Artificial photosynthesis (Washington, D.C.)","volume":"1 4","pages":"174-187"},"PeriodicalIF":0.0,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12302070/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144746691","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Tuning the Photocatalytic CO₂ Reduction through para-Substituents in Bipyridyl Rhenium Complexes. 通过对取代基调整联吡啶铼配合物的光催化CO2还原。

Artificial photosynthesis (Washington, D.C.) Pub Date : 2025-02-19 eCollection Date: 2025-09-25 DOI: 10.1021/aps.4c00026

Andressa V Müller, Wendel M Wierzba, Luis G A do Nascimento, Javier J Concepcion, Sofia Nikolaou, Dmitry E Polyansky, Andre S Polo

{"title":"Tuning the Photocatalytic CO2 Reduction through para-Substituents in Bipyridyl Rhenium Complexes.","authors":"Andressa V Müller, Wendel M Wierzba, Luis G A do Nascimento, Javier J Concepcion, Sofia Nikolaou, Dmitry E Polyansky, Andre S Polo","doi":"10.1021/aps.4c00026","DOIUrl":"10.1021/aps.4c00026","url":null,"abstract":"Six fac-[Re-(NN)-(CO)3Cl] complexes, where NN is a 2,2'-bipyridine ligand with systematically varied electron-donating or -withdrawing groups at the 4,4' positions, were explored as photocatalysts for CO2 reduction to CO. The light absorption, redox potentials, and excited-state dynamics of the complexes, as well as the reactivity and stability of key catalysis intermediates, were correlated with the Hammett constants (σp) of the substituents, revealing their impact on the photocatalytic activity. Electron-donating substituents, such as -OCH3 and -CH3, resulted in slower excited-state quenching by sacrificial electron donors in comparison to the unsubstituted complex, but their corresponding one-electron-reduced species (OERS) reacted quickly with CO2. On the other hand, electron-withdrawing substituents, such as -Br, -COOH, and -CO2CH3, resulted in more favorable and faster reductive quenching, but at the cost of slower reactivity of the OERS. A comparison of the catalytic activity of the complexes employing two different sacrificial electron donors displayed how the interplay of these factors affects the CO2 reduction performance and how photocatalysis can be controlled by strategic manipulation of both the ligand environment and the reaction conditions.","PeriodicalId":520501,"journal":{"name":"Artificial photosynthesis (Washington, D.C.)","volume":"1 5","pages":"214-225"},"PeriodicalIF":0.0,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12478854/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145202851","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cobalt-Loaded Carbon Nitride Demonstrates Enhanced Photocatalytic Production of H₂ from Lignocellulosic Biomass Components. 负载钴的氮化碳证明了从木质纤维素生物质组分中增强光催化生产H2。

Artificial photosynthesis (Washington, D.C.) Pub Date : 2024-09-02 eCollection Date: 2025-01-23 DOI: 10.1021/aps.4c00007

Mitchell Beckedorf, Jenna Holland, Robert Godin

{"title":"Cobalt-Loaded Carbon Nitride Demonstrates Enhanced Photocatalytic Production of H2 from Lignocellulosic Biomass Components.","authors":"Mitchell Beckedorf, Jenna Holland, Robert Godin","doi":"10.1021/aps.4c00007","DOIUrl":"10.1021/aps.4c00007","url":null,"abstract":"Photocatalytic production of hydrogen (H2) from biomass is a promising avenue for advancing sustainable energy generation. We prepared carbon nitride (CN x ) with cobalt (Co) as an oxidation cocatalyst (denoted CN x /Co) to improve photocatalytic H2 production through photoreforming components of lignocellulosic biomass under visual light irradiation. CN x /Co was synthesized by loading Co onto preformed CN x through a straightforward thermal deposition. The thermal loading of Co at 450 °C led to the formation of a mixed valence CoO x , which shifted Co2+ character to Co3+ over the course of the hydrogen evolution reaction (HER). Compared to CN x without Co, our materials with 0.3 and 0.6 wt % Co demonstrate twice the apparent quantum yield (AQY) for H2 production under irradiation at 405 nm using glucose as a sacrificial electron donor (3.0% and 2.8%, respectively, vs 1.4%). Time-resolved spectroscopic investigations indicate that the Co extracts charges in the subnanosecond time scale and promotes the formation of beneficial long-lived charges. Impressively, some photocatalytic activity is observed when using the robust polymers of cellulose and lignin as the oxidation substrates (0.2 and 0.1% AQY, respectively). The ability to oxidize abundant biomass without extensive prepreparation is promising for waste upcycling applications.","PeriodicalId":520501,"journal":{"name":"Artificial photosynthesis (Washington, D.C.)","volume":"1 1","pages":"50-62"},"PeriodicalIF":0.0,"publicationDate":"2024-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11783807/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813339","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0