Review
Chemistry, Physical
Kejia Wu, Minglong Cao, Qiang Zeng, Xuehui Li
Summary: Lignin, as a major component of woody biomass, is a natural organic polymer and the only abundant natural renewable resource with aromatic nucleus. Chemical catalysis induced depolymerization and photocatalysis and electrocatalysis are effective methods for lignin utilization. In this contribution, the radical and (photo)electron transfer induced reaction mechanisms of lignin depolymerization are discussed, along with the challenges and opportunities of photo(electro)catalysis in lignin valorization.
GREEN ENERGY & ENVIRONMENT
(2023)
Article
Chemistry, Multidisciplinary
Alafate Adili, Angie B. Korpusik, Daniel Seidel, Brent S. Sumerlin
Summary: Visible light-mediated direct decarboxylation is a versatile technique for the synthesis of functional materials with tailored compositions and properties. This process allows for the generation of carbon-centered radicals in polymer chains without the need for preactivation of acid groups. It can be used to obtain challenging copolymers and trigger degradation of polymer backbones.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Multidisciplinary
Fabian Eisenreich
Summary: Shaping a sustainable future is closely tied to advanced plastic recycling technologies. Low global recycling rates result in the incineration or landfill disposal of post-consumer plastics, causing severe environmental risks and a loss of chemical resources. Recent breakthroughs in photocatalytic methods offer a solution by converting polymers into valuable organic molecules under environmentally benign conditions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Stefan Simic, Migle Jakstaite, Wilhelm T. . S. Huck, Christoph K. Winkler, Wolfgang Kroutil
Summary: The challenges of light-dependent biocatalytic transformations of lipophilic substrates in aqueous media are addressed through continuous flow reactions. The immobilization of the catalyst on a carrier or using a homogeneous system is determined by the photostability of the catalyst. Homogeneous conditions in the CvFAP-catalyzed photodecarboxylation of palmitic acid achieved a high space-time yield, demonstrating the advantage of continuous flow for photobiocatalytic processes.
Article
Chemistry, Multidisciplinary
Marcia G. A. da Cruz, Robin Gueret, Jianhong Chen, Jedrzej Piatek, Bjoern Beele, Mika H. Sipponen, Marcella Frauscher, Serhiy Budnyk, Bruno V. M. Rodrigues, Adam Slabon
Summary: Breaking down lignin into smaller units is crucial for generating high value-added products. However, finding an environmentally friendly way to dissolve this complex plant polyphenol has always been a challenge. In this study, levulinic acid was used as a medium to reductively electrochemically depolymerize lignin, resulting in the formation of lignin-derived monomers and dimers. The depolymerized lignin was further evaluated as an anti-corrosion coating, exhibiting enhanced electrochemical stability for metals.
Editorial Material
Chemistry, Multidisciplinary
Bruno V. M. Rodrigues, Adam Slabon
Summary: Breaking down lignin into smaller units is crucial for producing high value-added products. However, finding an environmentally friendly way to dissolve this complex plant polyphenol often poses a challenge. Levulinic acid, which is generated during the hydrothermal processing of lignocellulosic biomass, has been found to effectively dissolve lignin. This study demonstrates the reductive electrochemical depolymerization of lignin using levulinic acid as a medium and copper as an electrocatalyst. After depolymerization, lignin-derived monomers and dimers with predominance of aryl ether and phenolic groups were observed. The depolymerized lignin also showed improved electrochemical stability when used as an anti-corrosion coating. This research highlights a simple approach to produce high value-added compounds or tailored biobased materials from biomass waste in a biomass-based solvent.
Review
Chemistry, Multidisciplinary
Arnaud Thevenon, Ina Vollmer
Summary: Efficient chemical depolymerization of waste polyolefins to monomers is still a challenge, but it can help prevent further waste accumulation and generate economic benefits. A recent study by Conk et al. successfully converted polyethylene (PE) into propylene using a tandem catalysis approach, with yields as high as 87%. This proof of concept opens up possibilities for future research on catalyst optimization, process design, and compatibility with contaminated and multi-polymer waste streams.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Viet D. Nguyen, Ramon Trevino, Samuel G. Greco, Hadi D. Arman, Oleg V. Larionov
Summary: Dual catalytic systems involving photocatalytic activation and transition metal-catalyzed steps have enabled innovative approaches to the construction of carbon-carbon and carbon-heteroatom bonds. This study reports a dual catalytic process that enables the direct conversion of carboxylic acids to important synthetic intermediates using a three-component decarboxysulfonylative cross-coupling. Detailed mechanistic and computational studies revealed the roles of different catalysts and ions in channeling the reaction.
Article
Chemistry, Multidisciplinary
Xiangze Du, Yong Peng, Josep Albero, Dan Li, Changwei Hu, Hermenegildo Garcia
Summary: This study investigated the photocatalytic decarboxylation of octanoic acid using a series of modified TiO2 catalysts to produce mixtures of n-heptane and tetradecane. The optimal NaBH4 treatment was found to enhance the photocatalytic activity, leading to almost complete conversion of octanoic acid and high selectivity towards n-heptane and tetradecane. These results demonstrate the potential of photocatalytic decarboxylation for the production of synthetic fuels from biomass under mild conditions.
Review
Energy & Fuels
Liquan Jing, Yuanguo Xu, Huaming Li, Ian D. Gates, Jinguang Hu
Summary: This article reviews the synthesis strategies, catalytic enhancement mechanisms, and catalytic applications of MoSx, discussing its current limitations and future research directions.
Article
Chemistry, Physical
Chuanhao Li, Tong Song, Cong Xie, Wenbin Shi, Dan Wang, Ping Yang
Summary: This paper demonstrates the synthesis of high-quality thin g-C3N4 homojunctions by controlling precursor components during the seed growth process. The resulting samples showed changes in microstructure, band gap, and photoelectrochemical properties. Photocatalytic activities were tested through H2 generation and the photodegradation of Rhodamine B (Rh B). The formation of homojunctions improves the photoelectrocatalytic activities.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Organic
Euan B. McLean, David T. Mooney, David J. Burns, Ai-Lan Lee
Summary: A mild and inexpensive method for direct hydrodecarboxylation of aliphatic carboxylic acids has been developed, which does not require metals, light, or catalysts, making the protocol operationally simple and more sustainable.
Article
Chemistry, Physical
Feifei Wang, Ruipeng Ou, Hongbin Yu, Ying Lu, Jiao Qu, Suiyi Zhu, Leilei Zhang, Mingxin Huo
Summary: By integrating g-C3N4 nanosheets with alpha-Fe2O3 nanorod arrays and applying them for the photoelectrocatalytic degradation of PNP, this study achieved the highest removal efficiency for pollutants.
APPLIED SURFACE SCIENCE
(2021)
Review
Biochemistry & Molecular Biology
Rabia Ayub, Ahmad Raheel
Summary: Lignocellulosic biomass is a renewable resource with great potential for the production of high-value chemicals. Electrocatalytic depolymerization of lignocellulosic biomass offers a sustainable and economically viable approach to biomass transformation technology.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Chemistry, Multidisciplinary
Hong T. Duong, Yinqi Wu, Alexander Sutor, Bastien O. Burek, Frank Hollmann, Jonathan Z. Bloh
Summary: The study shows that wirelessly powered LEDs can effectively enhance the photobiosynthetic production of diesel alkanes from renewable fatty acids.
Article
Chemistry, Multidisciplinary
Chanon Pornrungroj, Virgil Andrei, Motiar Rahaman, Chawit Uswachoke, Hannah J. Joyce, Dominic S. Wright, Erwin Reisner
Summary: The integrated device combines PEC water splitting and electrolyzer functions, operating during the day with solar energy and at night with electricity to increase energy efficiency.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Review
Chemistry, Physical
Soma Vesztergom, Abhijit Dutta, Motiar Rahaman, Kiran Kiran, Ivan Zelocualtecatl Montiel, Peter Broekmann
Summary: The electrochemical deposition of metal foams around co-generated hydrogen bubbles that act as templates for the deposition is a promising, cheap and simple approach to the fabrication of new electrocatalyst materials. Metal foams obtained by dynamic hydrogen bubble templating offer an intrinsically high electrical conductance with an open porous structure that enables the fast transport of gases and liquids. The confined space within the pores of these metal foams may act as small reactors that can harbor reactions not possible at an open electrode interface.
Article
Electrochemistry
Eva Vaneckova, Milan Bousa, Violetta Shestivska, Jiri Kubista, Pavel Moreno-Garcia, Peter Broekmann, Motiar Rahaman, Martin Zlamal, Jan Heyda, Milan Bernauer, Tana Sebechlebska, Viliam Kolivoska
Summary: This study utilized 3D printing to manufacture catalysts for the electrochemical reduction of CO2 with promising results. Functionalized carbon nanotube-based electrodes printed by fused deposition modeling demonstrated performance characteristics approaching those of planar interfaces. The activity of the catalysts was inspected by monitoring the concentration of formate ions in the saturated CO2 solution, showing comparable efficiency to conventionally prepared micro-structured copper catalysts.
Article
Chemistry, Multidisciplinary
Subhajit Bhattacharjee, Virgil Andrei, Chanon Pornrungroj, Motiar Rahaman, Christian M. Pichler, Erwin Reisner
Summary: A perovskite-based photoelectrochemical device is reported to produce H-2 fuel and reform waste substrates with high product selectivity and formation rates, utilizing an oxidation catalyst to generate value-added products. The device shows significantly higher activity compared to conventional photoreforming systems and offers versatility in treating various waste streams. This PEC platform demonstrates potential as a commercially viable alternative for waste utilization.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Review
Chemistry, Multidisciplinary
Xinsheng Dong, Subhajit Bhattacharjee, Chonghuan Zhang, Fang Chai
Summary: Titanium carbides are promising materials for removing toxic HMIs and radionuclides from wastewater due to their hydrophilicity, controllable surface charge, specific active groups, and high radiation stability. Research has focused on developing functional titanium carbide composite materials to enhance adsorption performance and overcome limitations of conventional nanomaterials. The evolution of titanium carbide-based adsorbents from 2D nanosheets to a variety of composite materials and 3D architectures has been summarized, along with practical methods for design and synthesis. Adsorption mechanisms and potential applications of these surface-modified composite materials are discussed, highlighting the challenges and prospects for future development in metal ion adsorption.
ADVANCED MATERIALS INTERFACES
(2021)
Article
Chemistry, Physical
Virgil Andrei, Robert A. Jagt, Motiar Rahaman, Leonardo Lari, Vlado K. Lazarov, Judith L. MacManus-Driscoll, Robert L. Z. Hoye, Erwin Reisner
Summary: In this study, photocathodes with long-lasting H2 evolution activity were demonstrated by integrating a BiOI light absorber into a robust, oxide-based architecture with a graphite paste conductive encapsulant. Multiple-pixel devices were introduced as an innovative design principle for PEC systems, showing superior photocurrents, onset biases, and stability compared to conventional single-pixel devices.
Article
Chemistry, Physical
Christian M. Pichler, Subhajit Bhattacharjee, Erwin Lam, Lin Su, Alberto Collauto, Maxie M. Roessler, Samuel J. Cobb, Vivek M. Badiani, Motiar Rahaman, Erwin Reisner
Summary: This study demonstrates that ethylene can be produced through the electrocatalytic oxidative decarboxylation of succinic acid, offering an environmentally friendly route. The research provides insights into the mechanism of the reaction and establishes a two-step bio-electrochemical process for ethylene production using succinic acid sourced from food waste.
Article
Materials Science, Coatings & Films
Norica Godja, Luka Payrits, Markus Ostermann, Andreas Schindel, Markus Valtiner, Christian M. Pichler
Summary: Magnesium- or Aluminium based lightweight alloys are increasingly used in the automotive sector. Plasma electrolytic oxidation (PEO) can efficiently form protective layers on these lightweight alloy materials to ensure corrosion protection. This study investigates the feasibility of using the PEO process for joined Al-alloy and Mg-alloy materials and evaluates the compatibility with subsequent cathodic dip coating (CDC) processes and the corrosion resistance of the coated materials. The results demonstrate that both magnesium and aluminum alloys can be subjected to the PEO process after being joined, resulting in effective protective layer formation on both materials. The joined and PEO treated materials also exhibit excellent compatibility with the cathodic dip coating process and enhanced corrosion resistance.
SURFACE & COATINGS TECHNOLOGY
(2023)
Article
Energy & Fuels
Motiar Rahaman, Virgil Andrei, Demelza Wright, Erwin Lam, Chanon Pornrungroj, Subhajit Bhattacharjee, Christian M. Pichler, Heather F. Greer, Jeremy J. Baumberg, Erwin Reisner
Summary: The synthesis of high-energy-density liquid fuels from CO2 and H2O using sunlight has the potential to create a circular economy. A new artificial leaf device, integrated with a copper-palladium catalyst and perovskite-BiVO4 tandem light absorbers, has successfully produced multi-carbon alcohols through CO2 reduction and water oxidation. This study demonstrates the direct production of complex alcohols from CO2 over an artificial leaf, using sunlight as the only energy source.
Review
Chemistry, Physical
Christian M. Pichler
Summary: The chemical industry is actively promoting the use of alternative feedstocks to replace fossil resources and implementing more sustainable production routes. Waste feedstocks are of particular interest due to the principles of circular economy. However, waste feedstocks have complex structures, making it challenging to convert them into defined chemical products. Coupled catalytic processes are a viable solution to enable the conversion of waste feedstocks into value-added chemicals. This review discusses different strategies for converting waste substrates into value-added chemicals using process couplings, including electrochemical reactions. Such coupled processes are of great importance in transforming the chemical industry towards sustainable processes based on the principles of circular economy. Converting waste substrates into value-added chemical products is a promising pathway for implementing circular economy principles and replacing fossil feedstocks in the chemical industry.
Article
Chemistry, Physical
Maria Wolfsgruber, Prathamesh Patil, Christian M. Pichler, Robert H. Bischof, Serhiy Budnyk, Christian Paulik, Bruno V. M. Rodrigues, Adam Slabon
Summary: The electrocatalytic conversion of gluconic acid, an aldonic acid, into fermentable carbohydrates using silver as an electrocatalyst is a sustainable strategy for the valorization of spent sulfite liquor. This discovery highlights the potential for merging electrocatalysis and biorefinery concepts to create a bioelectrorefinery for side stream valorization, which is crucial for a bio-circular-green economy.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Biotechnology & Applied Microbiology
Muhammad Adeel Ashraf, Markus Valtiner, Aleksandra Gavrilovic-Wohlmuther, Juliane Kampichler, Christian M. Pichler
Summary: Metallic zirconium has potential applications in engineering and corrosive industries. Ionic liquids are suitable for electrochemical reactions of zirconium. The interaction between ionic liquids and zirconium precursors influences the diffusion properties of zirconium.
FRONTIERS IN CHEMICAL ENGINEERING
(2022)