Article
Chemistry, Physical
Lei Fang, Gaozhang Gou, Jin Shang, Mingxian Liu, Qinfen Gu, Liangchun Li
Summary: Covalent triazine frameworks (CTFs) can form versatile metal-N single-atom coordination sites as promising catalytic centers. A five-step strategy involving spin states has been established for hierarchical high-throughput screening of M/CTFs (M = Transition metal) as excellent catalysts for nitrogen reduction reaction (NRR). Among the potential candidates, Cr/CTF shows excellent performance for nitrogen fixation with strong inhibition of hydrogen evolution reaction (HER) and good thermodynamic stability, narrow band gap, moderate adsorption energy, large activation energy, and theoretical Faradaic efficiency of 100%.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Article
Chemistry, Physical
Lu Wang, Lin Wang, Saifei Yuan, Liping Song, Hao Ren, Yuankang Xu, Manman He, Yuheng Zhang, Hang Wang, Yichao Huang, Tong Wei, Jiangwei Zhang, Yuichiro Himeda, Zhuangjun Fan
Summary: This study presents an in situ covalent-bonding strategy to enhance the selectivity and activity of photocatalysts for CO2 reduction. The incorporation of Ru-N-2 units into the conjugated covalent triazine frameworks (CTFs) improves charge separation and stabilizes the catalyst, resulting in a high solar-to-formate conversion rate and selectivity. Experimental and computational evidence indicate that the H2O-substituted Ru-N-2 unit is the newly discovered active center for efficient photocatalysis.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Nanoscience & Nanotechnology
Dmitri A. Bulushev, Fedor S. Golub, Svetlana Trubina, Valentina V. Zvereva, Lyubov G. Bulusheva, Evgeny Y. Gerasimov, Miriam Navlani-Garcia, Anna D. Krot, Himanshu Sekhar Jena
Summary: In this study, we synthesized single-atom Pd catalysts supported on different materials and tested their catalytic performance in formic acid decomposition for hydrogen production. The Pd/CTF-1 catalyst showed the highest performance, while the Pd/bipyCTF catalyst exhibited very high selectivity at higher temperatures.
ACS APPLIED NANO MATERIALS
(2022)
Article
Chemistry, Physical
Chaonan Jin, Ning Li, En Lin, Xuepeng Chen, Ting Wang, Yan Wang, Mingfang Yang, Wansheng Liu, Jiangyue Yu, Zhenjie Zhang, Yao Chen
Summary: This study developed a photoenzymatic platform for asymmetric catalysis by immobilizing wheat germ lipase (WGL) onto rationally designed photocatalytic porphyrinic covalent organic frameworks (COFs). The WGL@COFs photobiocatalysts demonstrated high enzymatic activity and good operational stability, and exhibited excellent performance for an enantioselective Mannich reaction under visible light irradiation. This work provides a general and efficient strategy for fabricating photobiocatalysts that enable highly efficient photoenzymatic asymmetric catalysis using COFs as photocatalytic platforms for enzyme immobilization.
Article
Chemistry, Multidisciplinary
J. Chen, G. Li, N. Lu, H. Lin, S. Zhou, F. Liu
Summary: In this study, a nanospatial separation strategy for covalent triazine frameworks (CTFs) was developed to improve their photocatalytic efficiency. By incorporating single-atom cobalt (Co) into CTF-1 nanosheets, the obtained Co/CTF-1 exhibited significantly enhanced efficiency for pollutant photodegradation. The nanospatial separation of charge carriers achieved by the Co single atoms as oxidation centers resulted in improved photo-exciton dissociation and narrow bandgap.
MATERIALS TODAY CHEMISTRY
(2022)
Article
Nanoscience & Nanotechnology
Sara Abednatanzi, Parviz Gohari Derakhshandeh, Sasanka Dalapati, Savita K. P. Veerapandian, Anne-Claire Froissart, Jan Dirk Epping, Rino Morent, Nathalie De Geyter, Pascal Van der Voort
Summary: A robust nanoporous covalent triazine framework has been developed as a metal-free catalyst for the green chemoselective reduction of nitroarenes.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Chao Zhu, Lun Lu, Qile Fang, Shuang Song, Baoliang Chen, Yi Shen
Summary: In this study, a single-atom Ti-loaded covalent organic framework (Ti-1/CTF) was constructed and demonstrated to have great potential in the adsorption and photocatalytic degradation of organic pollutants. The essential role of the electronic spin state in regulating the material's activity was proven. The spin-polarized Ti-1-N-3/CTF-10 showed enhanced adsorption capacity and degradation kinetics for a specific pollutant, along with long-term stability and favorable cost-effectiveness in natural water applications.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Juan Wang, Zhihua Zhang, Yangyang Li, Yuanyuan Qu, Yongqiang Li, Weifeng Li, Mingwen Zhao
Summary: This study investigates the use of transition-metal atoms anchored to two-dimensional covalent-organic frameworks for single-atom catalysis in ammonia synthesis. Through a screening process, WPc-TFPN is identified as the best SAC for nitrogen reduction reaction with a low limiting potential of -0.19 V, and multiple-level descriptors are developed to uncover the origins of NRR activity.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Materials Science, Multidisciplinary
Yang Li, Yuanzhe Tang, Jian Li, Yanjiao Chang, Hongliang Huang, Chongli Zhong
Summary: The study explores the effects of stacking manner of 2D semiconductor on photocatalytic hydrogen production by fabricating two novel covalent triazine polymers (CTP). The results indicate that the compact CTP-TG-1 shows significantly higher photocatalytic activity compared to the incompact CTP-TG-2 due to faster charge-carrier transport. Furthermore, the design and synthesis of other CTPs further confirm the significant contribution of 2D stacking manner on photocatalytic hydrogen production.
JOURNAL OF MATERIALS SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Ruixue Sun, Xiaoyan Wang, Xuepeng Wang, Bien Tan
Summary: This research reports the design and synthesis of two 3D crystalline CTFs with moderate crystallinity, relatively large surface area, and high CO2 uptake capacity. These 3D CTFs exhibit ultrastability and provide a synthetic strategy and structural basis for expanding practical applications of CTF materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Nanoscience & Nanotechnology
Dmitri A. Bulushev, Fedor S. Golub, Svetlana V. Trubina, Valentina V. Zvereva, Evgeny Y. Gerasimov, Igor P. Prosvirin, Miriam Navlani-Garcia, Himanshu Sekhar Jena
Summary: Covalent triazine frameworks (CTF) have been used as supports for metal catalysts, and the nature of the CTF support can influence the catalytic properties. In this study, Pd catalysts supported on hatnCTF and acacCTF were compared with a Pd/g-C3N4 catalyst for formic acid decomposition. The Pd/hatnCTF catalyst showed significantly higher activity, attributed to single-atom Pd2+-C1N3 sites as the main active species.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Jing Zhang, Yuping Xu, Maowen Lan, Xiaodong Wang, Ning Fu, Zhenglong Yang
Summary: This study reports a refined catalyst obtained from CTF@MOF-x, which exhibits high oxygen reduction reaction (ORR) activity and excellent durability, providing new opportunities for CTF-derived carbon-based electrocatalysts to achieve high ORR performance.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Physical
Chengpeng Liu, Zhen Li, Huifang Liu, Jing Dong, Yingnan Chi, Changwen Hu
Summary: In this study, immobilized and active PMo12@CTF material with amphiphilic surface and excellent recyclability was successfully synthesized. The PMo12@CTF exhibited high catalytic activity and stability in the oxidative desulfurization of diesel fuel.
Article
Chemistry, Multidisciplinary
Yunlong Zheng, Sainan Zhang, Jinbiao Guo, Ruixuan Shi, Jiangyue Yu, Kaipeng Li, Ning Li, Zhenjie Zhang, Yao Chen
Summary: Enzyme immobilization is crucial for large-scale biocatalytic processes. This study presents a green and scalable approach to prepare high-performance biocatalysts through the assembly of enzymes with covalent organic frameworks. These biocatalysts have exceptional reusability and stability, making them efficient catalysts for important industrial reactions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Engineering, Environmental
Guocheng Huang, Qing Niu, Jiangwei Zhang, Huimin Huang, Qiaoshan Chen, Jinhong Bi, Ling Wu
Summary: This study presents an efficient photocatalytic CO2 reduction method by synthesizing Pt single atoms in a covalent triazine framework, resulting in high CH4 production. The presence of Pt single atoms improves CO2 adsorption and activation, accelerating the separation and transfer of photogenerated carriers, demonstrating superior photocatalytic performance and stability.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Jan Droenner, Peter Hausoul, Regina Palkovits, Matthias Eisenacher
Summary: This article focuses on the importance and challenges of the oxidation and cleavage steps in the production of phenol from cumene. Substituting sulfuric acid with heterogeneous catalysts is a widely explored approach to reduce energy consumption and waste production. Various types of heterogeneous catalysts have shown high yield and selectivity to phenol.
Review
Chemistry, Multidisciplinary
Dafeng Yan, Chalachew Mebrahtu, Shuangyin Wang, Regina Palkovits
Summary: Renewable H-2 production by water electrolysis has received much attention, but the energy consumption of conventional water electrolysis is high. This review summarizes the latest findings on innovative electrochemical strategies for H-2 production, including the use of redox mediators and alternative anodic reactions. The study also presents electrochemical H-2 production at both the cathode and anode, as well as the challenges and prospects for future development.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Joby Sebastian, Chalachew Mebrahtu, Regina Palkovits
Summary: Titania supported MoOx catalysts with varying surface densities of Mo were examined for the DODH reaction of 1,4-AHE. Isolated MoOx species were found to be more active than oligomeric/polymeric/crystalline MoOx species. The increase in Mo surface density resulted in strong acidity, favoring side reactions.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Marcelo Alves Favaro, Jin Yang, Daniel Ditz, Huseyin Kucukkececi, Mohammed H. Alkhurisi, Sebastian Bergwinkl, Arne Thomas, Elsje Alessandra Quadrelli, Regina Palkovits, Jerome Canivet, Florian M. Wisser
Summary: The ability to molecularly engineer materials is a powerful tool in improving heterogeneous catalysts. Porous organic polymers show promise as photocatalysts due to their high stability, excellent optoelectronic properties, and easy synthesis. This study presents a pyrene-based Covalent Triazine Framework (CTF) as an efficient photocatalyst for hydrogen evolution and carbon dioxide photoreduction, achieving significant production rates.
Article
Chemistry, Physical
Nina M. M. Sackers, Julia Nikodemus, Regina Palkovits, Philippe Sautet, Peter J. C. Hausoul
Summary: Despite previous kinetic studies, the mechanism of polyol hydrogenolysis on a Ru catalyst surface remains unclear. To gain insight into the mechanism, decomposition of methanol was investigated using a Ru/C catalyst and periodic DFT calculations on a Ru(0001) model surface. The results suggest that the surface is likely covered by hydrogen adsorbates during the experiments. On a clean Ru surface, a lower overall activation barrier is observed when fewer dehydrogenation steps occur before C-O bond cleavage in the substrate methanol. Transferring these findings to a hydrogen-saturated Ru surface, the pathway involving CH2O O-H formation and subsequent C-O cleavage is found to be the most favorable. This study highlights the significant influence of surface coverage on the activation barrier.
Article
Chemistry, Physical
Zonghang Li, Xiaohu Yi, Qiwen Wang, Yiming Li, Diantao Li, Regina Palkovits, Anna Katharina Beine, Chunguang Liu, Xiaohong Wang
Summary: This study achieved the direct conversion of cellulose to glycolic acid (GA) with a high yield of up to 75% using acidic/redox polyoxometalates (POMs) as catalysts in a one-pot reaction. Among the three POMs studied, H3PMo showed the most promising catalytic activity. The reaction pathway involves the activation of O2 and the crucial role of the reduced form [PMo10 VIMo2VO39]5- in GA production.
Editorial Material
Electrochemistry
Sonja D. Murtz, Florian Musialek, Norbert Pfander, Regina Palkovits
Summary: The Front Cover of this issue features the research findings of Prof. Regina Palkovits' group, showcasing an artistic close-up of an electrochemical cell demonstrating the oxidation of glycerol for efficient hydrogen production. The research article focuses on investigating the PtCu catalyst, which is visible in the zoom window in the upper part of the image. Read the full text of the Research Article at 10.1002/celc.202201114.
Article
Electrochemistry
Sonja D. Muertz, Florian Musialek, Norbert Pfaender, Regina Palkovits
Summary: In this study, PtCu/C catalysts with different metal ratios were investigated for glycerol electrooxidation in acidic media. The addition of Cu to the benchmark Pt/C catalyst increased the activity, productivity, as well as stability due to electronic and structural effects. The best performer Pt7Cu3/C showed an increase in mass activity of 56%. The combined methodology of comprehensive electrochemical characterization and application in electrolysis experiments provides a practical approach for improving glycerol assisted hydrogen production addressing major challenges such as CO poisoning and stability.
Article
Engineering, Environmental
Dongdong Chen, Abhishek Khetan, Huarong Lei, Valentina Rizzotto, Jia-Yue Yang, Jiuxing Jiang, Qiming Sun, Baoxiang Peng, Peirong Chen, Regina Palkovits, Daiqi Ye, Ulrich Simon
Summary: Reinforcing the dynamic motion of Cu sites in Cu-zeolites can significantly enhance the low-temperature reduction of NOx.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Electrochemistry
Maike Berger, Ioana M. Popa, Leila Negahdar, Stefan Palkovits, Bastian Kaufmann, Moritz Pilaski, Harry Hoster, Regina Palkovits
Summary: Nickel-iron layered double hydroxides (NiFe LDH) are efficient electrocatalysts for alkaline oxygen evolution reaction (OER). This study investigated the kinetic behavior of NiFe LDH catalysts with different intercalated anions using steady-state Tafel plots, impedance measurements, and reaction order plots. The results showed that intercalated anions affect the rate-determining steps and have a significant impact on the OER activity.
Article
Chemistry, Multidisciplinary
Micjel Chavez Morejon, Nils Kurig, Yannick S. Tschauder, Falk Harnisch, Regina Palkovits
Summary: This study elucidates key parameters allowing the electrochemical valorization of cellobiose, by creating value-added products by both, anodic oxidation, and cathodic reduction. The first electrochemical reduction of cellobiose to cellobitol was achieved in a divided cell using Pb as cathode, with a conversion rate of up to 49% but with long reaction times (over 26 h) and low coulombic efficiency (4%). The successful synthesis of cellobionic acid was demonstrated by mediated oxidation in an undivided electrochemical cell, with cellobiose oxidation highly selective, achieving up to 92% conversion at 48% coulombic efficiency when using a charge of 2 FE.
Article
Chemistry, Multidisciplinary
Justus Kuemper, Jerome Meyers, Rebecca Sebers, Nils Kurig, Regina Palkovits
Summary: Acrylonitrile is an important industrial chemical produced by the SOHIO process using fossil resources. To achieve sustainable production, a new route using biogenic substrates and electrolysis is proposed. The electrochemical synthesis of green acrylonitrile using d,l-glutamic acid as a substrate is achieved through electro-oxidative decarboxylation and non-Kolbe electrolysis, resulting in a two-step process with a maximum yield of 41.1%.
Article
Chemistry, Physical
Ariel A. Schoenberger Alvarez, Can Oezyalcin, Tom Padeken, Peter Mauermann, Bastian Lehrheuer, Stefan Sterlepper, Ahed Abouserie, Maurice Vennewald, Ulrich Simon, Regina Palkovits, Stefan Pischinger
Summary: This study investigates the influence of the NO2/NOx ratio on the formaldehyde-related effects using a copper exchanged chabazite type zeolite production catalyst under close to real conditions. The results show that formaldehyde preferentially reacts with NH3 under the chosen reaction conditions, leading to the formation of an intermediate that may undergo either catalytic decomposition or thermal decomposition depending on the NO2/NOx ratio. The presence of formaldehyde improves the NOx conversion efficiency at high NO2 fractions but deteriorates it at small NO2/NOx fractions.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Nina M. Sackers, Andree Iemhoff, Philippe Sautet, Regina Palkovits
Summary: Computational methods were used to investigate well-defined and characterized isolated Ir sites anchored on a covalent triazine framework (CTF) as a showcase for experimentally accessible single-site catalysts. The resting states of the catalyst species after immobilization and after reduction at 400 ? were identified, and they were found not to be the catalytically active species but rather pre-catalysts for the dehydrogenation of formic acid.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
