{"title":"Cobalt-Loaded Carbon Nitride Demonstrates Enhanced Photocatalytic Production of H<sub>2</sub> from Lignocellulosic Biomass Components.","authors":"Mitchell Beckedorf, Jenna Holland, Robert Godin","doi":"10.1021/aps.4c00007","DOIUrl":"10.1021/aps.4c00007","url":null,"abstract":"<p><p>Photocatalytic production of hydrogen (H<sub>2</sub>) from biomass is a promising avenue for advancing sustainable energy generation. We prepared carbon nitride (CN <sub><i>x</i></sub> ) with cobalt (Co) as an oxidation cocatalyst (denoted CN <sub><i>x</i></sub> /Co) to improve photocatalytic H<sub>2</sub> production through photoreforming components of lignocellulosic biomass under visual light irradiation. CN <sub><i>x</i></sub> /Co was synthesized by loading Co onto preformed CN <sub><i>x</i></sub> through a straightforward thermal deposition. The thermal loading of Co at 450 °C led to the formation of a mixed valence CoO <sub><i>x</i></sub> , which shifted Co<sup>2+</sup> character to Co<sup>3+</sup> over the course of the hydrogen evolution reaction (HER). Compared to CN <sub><i>x</i></sub> without Co, our materials with 0.3 and 0.6 wt % Co demonstrate twice the apparent quantum yield (AQY) for H<sub>2</sub> 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.</p>","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}
{"title":"Realizing the Use of Molecular Electrocatalysts for Conversion of CO<sub>2</sub> to Multielectron Products.","authors":"Arnab Ghatak, Idan Hod","doi":"10.1021/aps.4c00011","DOIUrl":"10.1021/aps.4c00011","url":null,"abstract":"","PeriodicalId":520501,"journal":{"name":"Artificial photosynthesis (Washington, D.C.)","volume":"1 1","pages":"1-3"},"PeriodicalIF":0.0,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11783806/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813344","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}
Cathal Burns, Elizabeth A Gibson, Linsey Fuller, Shafeer Kalathil
{"title":"Powering the Future: Unveiling the Secrets of Semiconductor Biointerfaces in Biohybrids for Semiartificial Photosynthesis.","authors":"Cathal Burns, Elizabeth A Gibson, Linsey Fuller, Shafeer Kalathil","doi":"10.1021/aps.4c00008","DOIUrl":"10.1021/aps.4c00008","url":null,"abstract":"<p><p>Developing technology for sustainable chemical and fuel production is a key focus of scientific research. Semiartificial photosynthesis is a promising approach, pairing \"electric microbes\" with artificial light absorbers (semiconductors) to convert N<sub>2</sub>, CO<sub>2</sub>, and water into value-added products using sunlight. Mimicking natural photosynthesis is done with semiconductors acting as electron donors or sinks for microbes. This method enables the production of multicarbon (C<sub>2</sub>+) chemicals (e.g., ethanol and caproic acid) and ammonia with high efficiency and selectivity. Despite significant progress, commercial-scale applications remain elusive due to fundamental challenges. This Review covers advances in semiartificial photosynthesis and highlights that there is no clear mechanistic understanding underpinning the production of chemicals using the combination of light, semiconductors, and microbes. Does the mechanism rely on H<sub>2</sub> uptake, do the microbes eat electrons directly from the light absorbers, or is it a combination of both? It focuses on overcoming bottlenecks using advanced spectroscopy, microscopy, and synthetic biology tools to study charge transfer kinetics between microbial cell membranes and semiconductors. Understanding this interaction is crucial for increasing solar-to-chemical (STC) efficiencies, necessary for industrial use. This Review also outlines future research directions and techniques to advance this field, aiming to achieve net-zero climate goals through multidisciplinary efforts.</p>","PeriodicalId":520501,"journal":{"name":"Artificial photosynthesis (Washington, D.C.)","volume":"1 1","pages":"27-49"},"PeriodicalIF":0.0,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11783821/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143813341","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}