Review
Biochemical Research Methods
Yoo Seok Lee, Rokas Gerulskis, Shelley D. Minteer
Summary: This review summarizes non-enzymatic and enzymatic electrochemical approaches for cofactor regeneration and discusses recent developments to solve major issues. Issues discussed include enzyme mutual inactivation, electron transfer rates, catalyst sustainability, product selectivity, and simplifying product purification. Recently reported remedies include heterogeneous metal catalysts and redox-polymer immobilized enzymatic systems.
CURRENT OPINION IN BIOTECHNOLOGY
(2022)
Article
Multidisciplinary Sciences
Feng Gao, Guangyu Liu, Aobo Chen, Yangguang Hu, Huihui Wang, Jiangyuan Pan, Jinglei Feng, Hongwei Zhang, Yujie Wang, Yuanzeng Min, Chao Gao, Yujie Xiong
Summary: Researchers have designed a programmable artificial photosynthetic cell that combines biological and non-biological components to enhance the regeneration of key cofactors. This approach provides a more versatile platform for customizing artificial photosynthetic cells to meet various demands for CO2 conversion.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Rui Lian, Lei Wang, Yang Gao, Jing Zhang, Qing Mei, Qizhao Wang
Summary: In this study, a ternary composite of CTU/CdS-P25 was successfully prepared by integrating commercial TiO2 particles into CdS grains and further integrating with a mixed-ligand-based metal organic framework (MOF) CTU. The resulting composite exhibited a broadened light absorption range and impressive photo-induced carrier transfer, leading to a significantly enhanced photocatalytic CO2 reduction performance.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Green & Sustainable Science & Technology
Han Chen, Yu Huang, Chong Sha, Jamile Mohammadi Moradian, Yang-Chun Yong, Zhen Fang
Summary: The conversion of CO2 into soluble formate is a promising strategy for carbon neutralization. Enzymatic CO2-to-formate processes have advantages such as high efficiency, selectivity, and mild reaction conditions. Different enzymes, including FDH, hydrogen-dependent CO2 reductase, and nitrogenase, as well as NADH-dependent and NADH-independent catalytic mechanisms, are summarized in this review. Challenges include costly sacrificial donors and low NADH regeneration efficiency, but new methods and systems offer opportunities to overcome these challenges. Enzymatic CO2-to-formate processes have versatile applications and the potential for bulk chemical biorefineries.
RENEWABLE & SUSTAINABLE ENERGY REVIEWS
(2023)
Article
Chemistry, Multidisciplinary
Gang Lin, Yuanyuan Zhang, Yutao Hua, Chunhui Zhang, Changchao Jia, Dianxing Ju, Cunming Yu, Peng Li, Jian Liu
Summary: In this study, a Rh-complex-based electron transfer unit was chemically attached onto the linker of MIL-125-NH2, enabling photo-induced electron transfer for NADH regeneration. The formate dehydrogenase was deposited onto the membrane, creating an efficient reaction interface and enhancing formic acid yield.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Li-Jun Zhao, Caimei Zhang, Shixin Zhang, Jiayang Chen, Xiaoyi Lv, Huijuan Su, Xun Sun, Toru Murayama, Caixia Qi
Summary: A novel dual-core drive transfer hydrogen heterogeneous catalysts Ir@CNT@ADH was developed by immobilizing alcohol dehydrogenase ADH and NADH-regenerated catalyst Pyren-Ir1 on carbon nanotubes. The catalyst showed significantly improved catalytic efficiency and recycling performance, holding great potential for the combined application of chemical catalysts and bioenzymes.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Applied
Pengye Zhang, Wenjin Dong, Yuanyuan Zhang, Li-Nan Zhao, Hualei Yuan, Chuanjun Wang, Wenshuo Wang, Hanxiao Wang, Hongyu Zhang, Jian Liu
Summary: This study proposes a novel immobilization method for photoenzyme-coupled catalysis, achieving efficient regeneration of NADH and CO2 reduction to formate. The method involves thermal polymerization of 2,2'-bipyridine-5,5'-diamine onto a polymeric carbon nitride framework, which allows for the integration of Rh complexes and N-doped graphene.
CHINESE JOURNAL OF CATALYSIS
(2023)
Article
Engineering, Chemical
Mengya Guo, Fengjuan Gu, Lingding Meng, Qiyong Liao, Zihui Meng, Wenfang Liu
Summary: This study investigates the reduction of CO2 to formaldehyde using a photo-enzyme coupled system. The optimal pH values and electron donors for the reactions are determined. Furthermore, the loading ratio of enzymes and the concentration of cofactors are optimized, and the stability of the system is examined. The results demonstrate the efficiency and stability of the photo-enzyme coupled system in producing formaldehyde from CO2.
SEPARATION AND PURIFICATION TECHNOLOGY
(2022)
Article
Chemistry, Physical
Kaiqi Xu, Athanasios Chatzitakis, Paul Hoff Backe, Qiushi Ruan, Junwang Tang, Frode Rise, Magnar Bjoras, Truls Norby
Summary: This study achieved stable and efficient reduction of CO2 to formate in a bio-hybrid PEC cell using a novel cathode and efficient regeneration mechanism, approaching the efficiency of natural photosynthesis.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Multidisciplinary
Zhibo Zhang, Jiahuan Tong, Xianglei Meng, Yingjun Cai, Shuangshuang Ma, Feng Huo, Jianquan Luo, Bao-Hua Xu, Suojiang Zhang, Manuel Pinelo
Summary: NADH is essential for enzymatic hydrogenation of CO2 to methanol, but its high costs limit its large-scale application. Photocatalytic reduction of NAD(+) to NADH is a promising solution utilizing solar energy. Efficient electron transfer from the photosensitizer to the catalyst is crucial for the success of NADH regeneration. Ionic porphyrin was identified as the most efficient photosensitizer for in situ NADH regeneration, leading to a sevenfold increase in methanol concentration when integrated with enzyme cascade reactions using a membrane support.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2021)
Article
Chemistry, Multidisciplinary
Xu Zhao, Sarah E. Cleary, Ceren Zor, Nicole Grobert, Holly A. Reeve, Kylie A. Vincent
Summary: Heterogeneous biocatalytic hydrogenation using metal catalysts and carbon supports for NADH recycling shows improved activity and selectivity in enantioselective C=X reduction reactions. By combining chemo- and biocatalysis on carbon supports, this method demonstrates a new way to efficiently produce bioactive NADH for high cofactor turnover numbers.
Article
Chemistry, Multidisciplinary
Hideki Ohtsu, Mikio Takaoka, Yosuke Tezuka, Kiyoshi Tsuge, Koji Tanaka
Summary: The study discovered an NAD(+)-type metal complex with oxidizing ability to convert alcohols to aldehydes and ketones, and successfully synthesized a novel zinc(II) complex with a C-C coupling ligand. Kinetic analysis based on absorption spectroscopic measurements revealed that the reaction proceeds through electron transfer followed by proton transfer mechanism.
CHEMICAL COMMUNICATIONS
(2021)
Article
Engineering, Environmental
Lihang Yan, Guanhua Liu, Jianqiao Liu, Jing Bai, Yaoxuan Li, Huaxun Chen, Liya Zhou, Jing Gao, Yanjun Jiang
Summary: This study developed a hierarchically porous structure by optimizing the pore structure of microporous UiO-66-NH2, which enhanced the enrichment of CO2 and the immobilization of formate dehydrogenase. The enzyme electrocatalytic system improved the CO2 reduction efficiency through the combination of CO2 enrichment and electrocatalytic NADH regeneration. The optimized catalytic system achieved a significantly higher formate yield compared to the free enzyme system.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Nanoscience & Nanotechnology
Pengye Zhang, Jundie Hu, Yangbin Shen, Xiaogang Yang, Jiafu Qu, Feng Du, Wei Sun, Chang Ming Li
Summary: By combining light with enzymes, a metal-free heterojunction of pyromellitic diimide/g-C3N4 (PDI/CN) with excellent visible light response was fabricated for efficient conversion of CO2 to formic acid. The unique photoenzymatic catalytic cascade system and heterointerface effect of PDI/CN contributed to the high selectivity and yield achieved. This work provides an efficient strategy and photocatalyst for the directional conversion of CO2 to formic acid.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Leonardo Tensi, Luca Rocchigiani, Gabriel Menendez Rodriguez, Edoardo Mosconi, Cristiano Zuccaccia, Filippo De Angelis, Alceo Macchioni
Summary: The reaction mechanism of nicotine amide dinucleotide hydrogenation (NAD(+) to NADH) catalyzed by Cp*Ir(pyridine-2-sulfonamidate) complexes in the presence of phosphonic acid has been elucidated. The enhanced performance of these catalysts stems from the hemilability of the pyridine ligand, which is displaced during P-H bond activation and facilitates the generation of the metal-hydride intermediate. Experimental results are supported by DFT calculations showing the importance of hydrogen bonding interactions in the activation of phosphite anions. Direct comparison between the unsubstituted catalyst and the 6-aminopyridine-2-sulfonamidate derivative reveals the molecular origin of the latter's superior performance, paving the way for the intelligent design of better catalysts for NADH regeneration.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Davide Michele Stefano Marcolongo, Francesco Nocito, Nicoletta Ditaranto, Roberto Comparelli, Michele Aresta, Angela Dibenedetto
Summary: This study reports the synthesis and characterization of mixed metal oxides as p,n-junction photocatalysts, and demonstrates the correlation between the preparation technique and the properties of the materials. The optical and electronic properties of the materials were evaluated using spectroscopic and characterization techniques.
Article
Chemistry, Physical
Chang Cheng, Bicheng Zhu, Bei Cheng, Wojciech Macyk, Linxi Wang, Jiaguo Yu
Summary: This study constructed a series of pyrene-alt-dibenzothiophene-S,S-dioxide (P16PySO)/tungsten trioxide (WO3) composites to investigate the mechanism of photocatalytic styrene oxidation under anaerobic and aerobic conditions. The S-scheme charge transfer pathway within P16PySO/WO3 was systematically analyzed. The results revealed that triplet oxygen (O-3(2)) could efficiently trap the energy of triplet excited P16PySO through an energy transfer process and convert to singlet oxygen (O-1(2)), which played an important role in styrene oxidation.
Article
Chemistry, Multidisciplinary
Anna Jakiminska, Kaja Spilarewicz, Wojciech Macyk
Summary: This work aims to revise the photocatalytic activity mechanism of the TiO2/Ag2O system in photocatalytic water splitting with methanol photoreforming. The transformation of Ag2O into AgNPs during photocatalytic water splitting/methanol photoreforming was studied using various techniques. The influence of AgNPs on the optoelectronic properties of TiO2 was analyzed, and the lack of efficient p-n junction between TiO2 and Ag2O was observed. Furthermore, the impact of chemical and structural changes on the production of CO and CO2 from methanol photoreforming was investigated.
NANOSCALE ADVANCES
(2023)
Article
Polymer Science
Tomasz Baran, Szymon Wojtyla
Summary: Strontium titanate, a ternary n-type semiconductor, has shown promise in photocatalytic applications such as degradation of organic pollutants or oxygen evolution reaction due to its high durability. However, its photoactivity is not high, leading to efforts in improving its efficiency, such as combining it with graphene oxide. In this study, SrTiO3/graphene oxide photomaterials were synthesized and characterized, providing important insights into charge separation efficiency, carrier transport, and photostability relevant to photocatalytic degradation of toluene.
JOURNAL OF INORGANIC AND ORGANOMETALLIC POLYMERS AND MATERIALS
(2023)
Article
Chemistry, Physical
Francesco Nocito, Marco Bortoluzzi, Michele Aresta, Angela Dibenedetto
Summary: This article presents interesting reactions between urea and biosourced diols, driven by cheap catalysts, which result in the elimination of ammonia and water. Various compounds, including cyclic carbonates, linear mono- and diurethanes, cyclic urethanes, and oligomeric urethanes, can be synthesized under mild conditions. ZnO and CeO2, as catalysts, exhibit different behavior in promoting ammonia or water elimination, with CeO2 being recoverable and reusable. CeO2 also facilitates the formation of oligo-urethanes through sequential diol-urea coupling.
Article
Green & Sustainable Science & Technology
Kamil Urbanek, Kaja Spilarewicz, Jiaguo Yu, Wojciech Macyk
Summary: This work designed an advanced photocatalytic system composed of titanium dioxide (P25) and mSFO (Sn-doped magnetite with Fe-doped cassiterite) for gas phase CO2 reduction. A synthesis route of mSFO composite was proposed, and the obtained material was characterized by various techniques. The mSFO/P25 system showed photocatalytic reduction ability of CO2 to CO, which was confirmed by the use of labeled carbon dioxide. The surface photovoltage and electrochemical measurements supported the S-scheme mechanism.
MATERIALS TODAY SUSTAINABILITY
(2023)
Article
Chemistry, Physical
Kasidid Yaemsunthorn, Wiktoria Adamowicz, Marcin Kobielusz, Wojciech Macyk
Summary: The photocatalytic selective reduction of 3-nitrophenol to 3-aminophenol was studied using titanium dioxide in different compositions. Both intrinsic and extrinsic parameters were found to affect the reaction progress, with intrinsic factors related to the chemical, structural, and electronic properties and extrinsic factors related to the reaction conditions. The analysis revealed that the performance of anatase and rutile materials varied due to differences in interfacial electron transfer, charge recombination, reduction driving force, and methanol photooxidation efficiency. The understanding of these factors could lead to the rational design of efficient and selective photocatalysts.
Editorial Material
Chemistry, Inorganic & Nuclear
Angela Dibenedetto, Alceo Macchioni
Summary: The CIRCC is an international consortium consisting of 17 universities and 75 research units in Italy. It focuses on developing new chemical reactions, catalytic systems, and their potential industrial applications. This article introduces the consortium to EurJIC readers and summarizes the scientific articles featured in the Institute Feature dedicated to CIRCC.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Review
Chemistry, Physical
Tetiana Tatarchuk, Liubov Soltys, Wojciech Macyk
Summary: The global development of industry and agriculture has led to the contamination of aquatic environments with pharmaceuticals. The uncontrolled release of pharmaceuticals into water poses a threat to human health and the environment. Adsorption with magnetic nanoparticles is an effective method for removing pharmaceuticals from wastewater. This comprehensive review focuses on the use of magnetic nanoparticles for the removal of antibiotics and nonsteroidal anti-inflammatory drugs from aqueous environments. The study discusses the interaction between the adsorbent and the adsorbate and summarizes the factors that affect adsorption efficiency.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Chemistry, Physical
Peiyu Hu, Guijie Liang, Bicheng Zhu, Wojciech Macyk, Jiaguo Yu, Feiyan Xu
Summary: Exploring photocatalysts for CO2 conversion is a promising approach for mitigating energy scarcity and environmental pollution. In this study, SnO2/Cs3Bi2Br9 heterojunctions were constructed to enhance CO2 photoreduction. The unique structure enabled efficient separation of photoexcited electron/hole pairs and demonstrated excellent selectivity for CH4 production.
Article
Chemistry, Physical
Ying He, Zhengpeng Yang, Jiaguo Yu, Difa Xu, Chengyuan Liu, Yang Pan, Wojciech Macyk, Feiyan Xu
Summary: In this study, WO3/In2O3 S-scheme heterojunction photocatalysts were developed for CO2 photoreduction. The unique S-scheme mechanism and efficient activation of CO2 molecules on the In2O3 surface resulted in enhanced CO2 photoreduction performance with 53.7% selectivity for CH4. Photocatalytic and CO2-reduction mechanisms, as well as the enhanced CH4-selectivity, were elucidated through various spectroscopy techniques and simulations.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Anna Jakiminska, Wojciech Macyk
Summary: This work presents the preparation of titanium dioxide polymorphs modified with metallic (Au and Ag) nanostructures of different sizes. The photocatalytic activity, photoelectrochemical properties, and electronic properties of these materials were examined. Moreover, it was established that the surface plasmon resonance phenomenon does not significantly enhance the photocatalytic activity of the materials, and the deposition of metallic nanostructures significantly alters the redox properties of the materials.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Kamil Urbanek, Anna Jakiminska, Kaja Spilarewicz, Wojciech Macyk
Summary: This work investigates the application of highly defective cobalt and copper tungstates for photocatalytic CO2 reduction. The synthesized materials were characterized and their behavior in photocatalytic reactions was studied. CuT/TiO2 mixture is found to be more effective than CoT/TiO2 due to lower recombination rates of charge carriers and the presence of more active centers.
APPLIED SURFACE SCIENCE ADVANCES
(2023)
Article
Chemistry, Multidisciplinary
Anna Jakiminska, Kaja Spilarewicz, Wojciech Macyk
Summary: This study investigates the influence of plasmonic (gold) and non-plasmonic (palladium) nanostructures on the photocatalytic activity and redox properties of titanium dioxide. The results show that palladium primarily determines the activity of modified materials, while the surface plasmon resonance of gold has no effect on the activity. Moreover, the nanostructures induce changes in the redox properties of the semiconductor, regardless of their plasmonic or non-plasmonic nature.
NANOSCALE ADVANCES
(2023)
