Article
Multidisciplinary Sciences
Shuo Zhang, Miao Li, Jiacheng Li, Qinan Song, Xiang Liu
Summary: Metal-organic framework-derived cobalt-doped Fe@Fe2O3 catalyst shows high efficiency in electrochemical nitrate reduction and ammonia production, providing an important strategy in the design of electrocatalysts.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Physical
Sharon Abner, Aicheng Chen
Summary: This study investigates the electrochemical reduction of CO2 using cobalt-oxide nanodendrites as catalysts, demonstrating their superior catalytic activity and providing insights into the reduction mechanism through in-situ FTIR analysis. The innovative approach offers potential for designing and developing advanced electrocatalysts for energy and environmental applications.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Physical
Charles B. Musgrave III, Yuyin Li, Zhengtang Luo, William A. Goddard III
Summary: This study focuses on the key challenges of strong CO adsorption and facile CO dimerization in electrochemical CO2 reduction towards multi-carbon (C2+) products. By immobilizing CoPc on a single-walled carbon nanotube, selective reduction of CO2 to methanol is achieved through molecular strain. Fe, Ru, Co, and Ir are identified as the best catalysts among 20 elements embedded in PcEx, and CoPcEx is found to be the most promising catalyst for efficiently converting CO to ethylene. The bimetallic IrCoPcEx catalyst is also examined and shows potential for this conversion.
Article
Chemistry, Multidisciplinary
Chang Liu, Zixun Yu, Fangxin She, Jiaxiang Chen, Fangzhou Liu, Jiangtao Qu, Julie M. Cairney, Chongchong Wu, Kailong Liu, Weijie Yang, Huiling Zheng, Yuan Chen, Hao Li, Li Wei
Summary: By constructing heterogeneous molecular catalysts using cobalt porphyrins and carbon nanotubes, the catalytic properties and activity were successfully modulated, resulting in sustainable production of hydrogen peroxide with high selectivity and activity.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Maykon L. Souza, Fabio H. B. Lima
Summary: Gold nanoparticles functionalized with dibenzyldithiocarbamate (DBDTC-Au NPs) were synthesized in the lab, displaying excellent electrocatalytic activity for the reduction of CO2 to CO. The strong bonding and stability of the DBDTC ligand on the Au nanoparticles played a crucial role in enhancing CO formation efficiency. Through online differential electrochemical mass spectrometry (DEMS) experiments and gas chromatography (GC) analysis, it was demonstrated that the DBDTC-Au catalyst achieved high faradaic efficiency and selectivity for CO production.
Article
Energy & Fuels
Bo Xiong, Jing Liu, Yingju Yang, Wei Liu, Man Chen, Hongcun Bai
Summary: In this study, a machine learning-assisted screening model combined with density functional theory (DFT) and electrochemical experiments is developed to explore efficient trimetallic electrocatalysts for carbon dioxide reduction. The study reveals that the group of doped elements in the periodic table is the most important descriptor of Cu-based trimetallic electrocatalysts, and the support vector regression algorithm has the best predictive performance. The prediction and experimental results demonstrate that PdPt@Cu exhibits the best electrocatalytic performance for the CO2 reduction reaction.
Review
Chemistry, Physical
Yongxia Shi, Man Hou, Junjun Li, Li Li, Zhicheng Zhang
Summary: Large amounts of CO2 gas have been emitted into the atmosphere through human activities, causing environmental problems. Developing and utilizing renewable clean energy is crucial to reduce CO2 emission. Electrochemical CO2 reduction reaction (CO2RR) is considered an effective approach to obtain valuable chemicals and fuels. Copper has been proven to be the only catalyst that can efficiently reduce CO2 to hydrocarbons and oxygenates. However, pure Cu has limitations for industrial-scale production. Cu-based tandem catalysts are a promising strategy for improving CO2RR performance.
ACTA PHYSICO-CHIMICA SINICA
(2022)
Article
Chemistry, Physical
Hee-il Nam, Kyoung Ryeol Park, Yong-Wook Choi, Hye-ji Sim, Keun Yong Sohn, Dong-Ha Lim
Summary: As the issue of responding to climate change becomes a global concern, CO2 utilization technologies have been extensively studied. Among them, electrochemical reduction of CO2 to CO coupled with renewable energy sources is considered the most promising approach. Expensive noble metals such as Ag and Au have been commonly used as electrocatalysts, but in this study, zinc-blende structured ZnS materials are explored as alternative materials due to their good CO selectivity and controllable composition or microstructures. The synthesized TA-ZnS electrocatalyst demonstrates excellent CO2ER performance with around 83% CO Faraday efficiency and suppression of hydrogen production, showing stability over a wide range of potential.
APPLIED SURFACE SCIENCE
(2023)
Article
Engineering, Environmental
Tong Shi, Dong Liu, Hao Feng, Ying Zhang, Qiang Li
Summary: This study investigates the evolution of electrode surface and CO2RR performance after surface modifications. The results show that the modified copper electrode forms a stable triple-phase interface, resulting in enhanced current density and reduced H2 production.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Narges Atrak, Ebrahim Tayyebi, Egill Skulason
Summary: Density functional theory calculations were used to investigate the effect of solvent on the stability of intermediates in CO2 reduction reaction on twelve rutile transition metal dioxide surfaces. It was found that co-adsorbed water can change the overpotentials for the formation of formic acid and methanol, shifting the selectivity towards formic acid. Different transition metal dioxides exhibit varying selectivity towards CO2 reduction products.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Yanling Qiu, Wenbin Xu, Pengfei Yao, Qiong Zheng, Huamin Zhang, Xianfeng Li
Summary: This study focuses on the electrochemical reduction of CO2 to valuable chemicals using Cu electrodes derived from Cu2O with predominant (111) facets. The optimized electrode shows high faradaic efficiency for HCOOH production, surpassing most reported Cu electrodes. The catalytic activity of unit active sites on Cu2O-derived Cu electrodes is found to be higher than that on blank Cu electrodes, with OCHO* production being favored in the presence of cetyltrimethylammonium bromide.
Article
Chemistry, Multidisciplinary
Shuanglin He, Yuhang Qing, Ping Zhang, Ying Xiong, Qianqian Wu, Yaping Zhang, Lin Chen, Fang Huang, Fei Li
Summary: A series of manganese polypyridine complexes were investigated as CO2 reduction electrocatalysts. The intramolecular proton tunneling distance significantly affected the selectivity of the CO2 reduction reaction, with a difference of approximately 0.3 angstroms. Catalysts with longer intramolecular proton tunneling distances favored proton binding to the [Mn-CO2] adduct, resulting in 100% selectivity for CO production. In contrast, catalysts with shorter distances showed a switch in product from CO to HCOOH with a selectivity of 86%.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Physical
Israr Masood ul Hasan, Luwei Peng, Jianfeng Mao, Ruinan He, Yongxia Wang, Jing Fu, Nengneng Xu, Jinli Qiao
Summary: The article discusses the progress and challenges of carbon-based metal-free catalysts in electrochemical CO2 reduction, aiming to provide insights for future research on more efficient low carbon-based fuels.
Article
Chemistry, Physical
Huimin Liu, Janis Timoshenko, Lichen Bai, Qinye Li, Martina Ruscher, Chenghua Sun, Beatriz Roldan Cuenya, Jingshan Luo
Summary: In this study, rhodium nanoflowers (Rh NFs) were designed as catalysts to reduce the overpotential required for electrocatalytic nitrate reduction to ammonia (NITRR), achieving efficient ammonia synthesis.
Article
Engineering, Environmental
Tianlun Ren, Kaili Ren, Mingzhen Wang, Mengying Liu, Ziqiang Wang, Hongjing Wang, Xiaonian Li, Liang Wang, You Xu
Summary: In this study, Cu nanowires with concave-convex surface Cu2+1O layers were prepared for efficient nitrate electroreduction to ammonia. The electronic interactions and interface effects between Cu and Cu2+1O contribute to the improved electroreduction ability over the Cu@Cu2+1O NWs. Tailoring surface/interface properties and atom structure can lead to highly efficient electrocatalysts for ammonia synthesis.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Cheng Chen, Zi-Jun Tang, Jia-Yi Li, Cong-Yi Du, Ting Ouyang, Kang Xiao, Zhao-Qing Liu
Summary: In situ growing transition metals on N-doped carbon by atomic doping presents a potential alternative to replace Pt-based catalysts for redox reactions. This study presents a simple synthetic strategy to fabricate a highly active and durable MnO modifying Co-N-x/C catalyst. The interphase engineering effectively controls the composition of the material, and the interaction between Co-N-x and MnO phase is also discussed. The resulting catalyst exhibits excellent electrocatalytic properties and durability in acidic and basic solutions.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Qiu-Ren Pan, Bi-Lin Lai, Li-Juan Huang, Yan-Nan Feng, Nan Li, Zhao-Qing Liu
Summary: In this study, a three-dimensional hierarchical porous copper, nitrogen, and boron codoped carbon catalyst was synthesized, which exhibited excellent oxygen reduction reaction (ORR) performance and stability. The introduction of boron atoms increased the electron density around the active site, promoting the efficiency of the ORR process and preventing demetallization. This research provides a new approach for the development of Cu-based ORR electrocatalysts and guidance for high-performance microbial fuel cells (MFCs) design.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Zepan Wang, Peiyuan Wu, Xubing Zou, Sheng Wang, Lei Du, Ting Ouyang, Zhao-Qing Liu
Summary: By partially replacing Co3+ with the more electro-negative Mn3+ ion at the octahedral site, a ternary Zn-Mn-Co spinel oxide is formed, leading to a significant increase in electrocatalytic oxygen reduction/evolution activity. Physical characterization and theoretical calculations show that bond competition plays a crucial role in regulating the cobalt valence state and the electrocatalytic activity. The partial replacement of Co3+ by Mn3+ effectively modulates the adjacent Co-O bond and induces the Jahn-Teller effect, resulting in a change in crystal structure and optimization of the binding strength with reaction intermediates. The Mn-substituted ZnMn1.4Co0.6O4/NCNTs exhibit higher electrocatalytic activity than ZnCo2O4/NCNTs and ZnMn2O4/NCNTs, indicating that the covalency of the Co-O bond determines the oxygen reduction reaction (ORR) activity of spinel ZnCo2O4. This study introduces the competition between adjacent Co-O and Mn-O bonds through the B-Oh-O-B-Oh edge-sharing geometry, demonstrating that ion substitution at octahedral sites with less electronegative cations can effectively enhance the electrocatalytic performance of cobalt-based spinel oxides.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Zehong Chen, Xinwen Peng, Zhongxin Chen, Tingzhen Li, Ren Zou, Ge Shi, Yongfa Huang, Peng Cui, Jian Yu, Yuling Chen, Xiao Chi, Kian Ping Loh, Zhaoqing Liu, Xuehui Li, Linxin Zhong, Jun Lu
Summary: The by-product of the papermaking industry, lignosulfonate, is used as a bioligand to produce single-atom catalysts (SACs) with highly active M-N-4-S sites (M represents Fe, Cu, and Co) through metal-nitrogen/sulfur coordination. This study demonstrates that the SACs produced have excellent catalytic performance in oxygen reduction and evolution reactions for Zn-air batteries, paving the way for the industrial production of cost-effective SACs in a sustainable manner.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Si -Tong Guo, Zi-Yuan Tang, Ting Liu, Ting Ouyang, Zhao-Qing Liu
Summary: In this study, a chlorine (Cl)-modified Cu2O/ZnO heterostructure photocathode (CCZO) with high CH4 faradaic efficiency (88.6%) and durability (over 5 h) is presented. The Cl ions in CCZO stabilize Cu2O against photo-corrosion and promote the hydrogenation of *CO intermediate, leading to the selective reduction of CO2 to CH4. The catalytic mechanism of CCZO in modulating the energy barrier of intermediate *CO combined with H+ is elucidated, providing a new idea for developing high selectivity and stable catalysts for CO2 reduction.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Multidisciplinary
Ge Shi, Xinwen Peng, Jiaming Zeng, Linxin Zhong, Yuan Sun, Wu Yang, Yu Lin Zhong, Yuxuan Zhu, Ren Zou, Shimelis Admassie, Zhaoqing Liu, Chuanfu Liu, Emmanuel I. Iwuoha, Jun Lu
Summary: Maintaining a steady affinity between gallium-based liquid metals and polymer binders is challenging for continuous mechanical deformation applications. In this study, a LM-initialized polyacrylamide-hemicellulose/EGaIn microdroplets hydrogel is developed as a multifunctional ink for 3D-printing self-standing scaffolds and anode hosts for Zn-ion batteries. The hydrogel acts as a framework for stress dissipation, allowing for recovery from structural damage caused by cyclic plating/stripping of Zn2+.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Jingjing Cai, Huijian Zhang, Lizhu Zhang, Yuqing Xiong, Ting Ouyang, Zhao-Qing Liu
Summary: The electronic structure of transition metal complexes can be modulated by replacing partial ions, which can lead to tuned electrocatalytic activity for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). However, the ORR activity of anion-modulated transition metal complexes is still unsatisfactory and it remains challenging to construct hetero-anionic structures. In this study, atomic doping strategy was used to prepare CuCo2O4-xSx/NC-2 (CCSO/NC-2) electrocatalysts, which showed excellent catalytic performance and durability for ORR and OER due to the partial substitution of S atoms for O in CCSO/NC-2. The introduction of S optimized the reaction kinetics and promoted electron redistribution.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Kang Xiao, Yifan Wang, Peiyuan Wu, Liping Hou, Zhao-Qing Liu
Summary: By incorporating F anions into the oxygen vacancies of spinel ZnCo2O4, the lattice oxidation mechanism (LOM) of oxygen evolution reaction (OER) has been triggered and the residual protonation has been balanced, leading to the stabilization of the catalyst structure.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Xiuying Li, Jiayue Hu, Yuepeng Deng, Tong Li, Zhao-Qing Liu, Zhu Wang
Summary: In this study, a Fenton-like catalyst with dual-photo-functional sites of iron phosphide (FeP) and Fe single atom-graphene oxide (Fe1-GO) nanocomposite was developed for the degradation of antibiotic tetracycline (TC) pollutants. The FeP/Fe1-GO catalyst exhibited significantly higher efficiency in TC degradation under visible light irradiation compared to single component catalysts. Moreover, the catalyst demonstrated excellent stability with 100 cycles of recycling and a wide pH range tolerance from 3-11. The study also provided insights into the TC degradation pathway and the toxicity of intermediate products.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Engineering, Environmental
Shangyu Hu, Yaxiong Zhan, Peilei Wang, Jingfei Yang, Fengxiu Wu, Meng Dan, Zhao-Qing Liu
Summary: The production of hydrogen peroxide (H2O2) through electrochemical oxygen reduction is a convenient and clean approach. A universal urotropine modified carbon-based catalyst was developed, which not only provides isolated O-2 active sites to protect OOH* from further splitting, but also excites the carbon nanotube matrix to produce abundant secondary O-2 active sites. Furthermore, the end-on type adsorption of O-2 on the excited secondary reactive sites can be stabilized by the hydrogen bond effect, leading to a significant increase in H2O2 productivity.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Inorganic & Nuclear
Zhilong Jiang, Weiya Liu, Jun Wang, Bangtang Chen, Zihao Wu, Fan Fu, Rui Miao, Ting Ouyang, Wenzhi Lv, Yongchao Huang, Die Liu, Zhao-Qing Liu, Mingzhao Chen, Pingshan Wang
Summary: The design and synthesis of two bipyridyl and terpyridyl ruthenium(II) building units L1 and L2 were explained, and two different triangle self-assembled supramolecules S1 and S2 were successfully synthesized. The study of S2 showed that it maintains high luminous performance at ambient temperature, opening up new possibilities for the rational molecular design of terpyridyl ruthenium fluorescent materials and catalytic functional materials.
INORGANIC CHEMISTRY
(2023)
Article
Polymer Science
Zhilang Liu, Zhaoqing Liu, Bo Shu, Cuixia Lian, Jialin Wu, Qing Wen, Jiahuan Wu, Zhuohong Yang, Wuyi Zhou, Yang Hu
Summary: Flexible and biodegradable polymer hydrogels are widely studied for biomedical applications, but achieving satisfactory mechanical performance, anti-swelling behavior, antibacterial activity and conductivity in one single hydrogel is still challenging. Researchers have developed a simple one-pot approach to prepare multiple-crosslinked PVA/PA-Fe hydrogels with favorable mechanical properties, anti-swelling behavior, antibacterial activity, and conductivity.
JOURNAL OF APPLIED POLYMER SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Si-Tong Guo, Yu-Wei Du, Huihua Luo, Ziyin Zhu, Ouyang Yang, Zhao-Qing Liu
Summary: Zn-based catalysts have great potential for CO2 reduction, and undercoordinated Zn sites can enhance CO production. However, the dynamic evolution and stability of Zn delta+ sites during CO2 reduction process are less explored. The study shows that Zn delta+ sites can suppress HER and HCOOH production to induce CO generation, and CeO2 nanotubes can stabilize Zn delta+ species.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Engineering, Environmental
Can-Wen Yu, Cong-Yi Du, Ting Ouyang, Xi-Ting Zhang, Zhao-Qing Liu
Summary: Physical structure change of catalysts based on the electronic metal-support interaction effects is a prospective strategy to enhance their catalytic performance. In this study, Ag and MnCo2O4 supported on N-doped carbon nanotubes were synthesized using a facile hydrothermal and photoreduction strategy, and exhibited enhanced performance for oxygen evolution reaction and oxygen reduction reaction. Theoretical calculations showed that the introduction of Ag optimized the adsorption properties and lowered the reaction activation energy, providing new insights for the fabrication of advanced oxygen electrocatalysts.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Jingwei Li, Zhengyi Huang, Cong Wang, Lei Tian, Xiaoqing Yang, Rongfu Zhou, Mohamed Nawfal Ghazzal, Zhao-Qing Liu
Summary: In this research, the efficient transfer of photoexcited carriers was achieved by introducing amorphous carbon into bandgap-broken heterojunctions. The formation of similar orbital energies enabled the migration of electrons and holes to the amorphous carbon, thereby enhancing carrier separation in the heterojunction. By controlling the relative amount of metal-O-C bonds at the interface, the charge transfer kinetics could be modulated, resulting in a significant increase in H2 generation. This strategy can be extended to other carbon allotropes, demonstrating its universality in optimizing charge transfer in broken-bandgap heterojunctions for photocatalytic H2 production.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
