Article
Chemistry, Physical
Jie Zhang, Thi Ha My Pham, Zhixiao Gao, Mo Li, Youngdon Ko, Loris Lombardo, Wen Zhao, Wen Luo, Andreas Zuttel
Summary: Metal complexes have been found to be selective and active catalysts for electrochemical CO2 reduction (CO2RR). Using in situ Raman, X-ray photoelectron spectroscopy, and advanced electron microscopy, researchers have discovered that copper phthalocyanine (CuPc) undergoes reconstruction during CO2RR. Further investigations have revealed that CuPc demetalates to Cu atoms, which then agglomerate to form Cu clusters and Cu nanoparticles (NPs). The size of the Cu NPs is highly dependent on experimental parameters, and the selectivity of multicarbon products is positively correlated with NP size. This study provides important insights for future applications of metal complex catalysts in CO2RR and inspires the design of advanced electrocatalysts for other electrochemical reactions.
Review
Chemistry, Multidisciplinary
Jinxian Wang, Danni Deng, Qiumei Wu, Mengjie Liu, Yuchao Wang, Jiabi Jiang, Xinran Zheng, Huanran Zheng, Yu Bai, Yingbi Chen, Xiang Xiong, Yongpeng Lei
Summary: This review summarizes the recent progress of atomically dispersed (AD) copper catalysts as a chemically tunable platform for electrochemical CO2 reduction (ECO2R). It discusses the dynamic evolution, catalytic performance, and mechanism of these catalysts, as well as the prospects and challenges in the field. The review aims to contribute to the rational design of AD copper catalysts with enhanced performance for ECO2R.
Article
Chemistry, Multidisciplinary
Michael R. R. Smith, Clare B. B. Martin, Sonia Arumuganainar, Ari Gilman, Bruce E. E. Koel, Michele L. L. Sarazen
Summary: Immobilization of porphyrin complexes into metal-organic frameworks enables high exposure of active sites for CO2 electroreduction. Well-dispersed iron-porphyrin-based MOF (PCN-222(Fe)) on carbon-based electrodes showed optimal turnover frequencies for CO2 reduction to CO. In situ Raman spectroscopy revealed the structure stability of PCN-222(Fe) and a stepwise electron transfer-proton transfer mechanism for CO2 electroreduction.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Benjamin P. Charnay, Zhihao Cui, Melissa A. Marx, Joseph Palazzo, Anne C. Co
Summary: This study investigates the electrochemical reduction of aldehydes to alcohols as a pathway for converting CO2 to alcohols. Experimental results support the proposed mechanism of reducing acetaldehyde and propionaldehyde to ethanol and 1-propanol on a Cu catalyst. Notably, acetaldehyde is selectively reduced to ethanol on Cu, but not on Au, as supported by both experimental observations and DFT calculations.
Article
Chemistry, Physical
Debolina Misra, Giovanni Di Liberto, Gianfranco Pacchioni
Summary: The electrochemical reduction of CO2 on single atom catalysts (SAC) is a promising but complex process that requires a deep understanding of each step. Most theoretical studies neglect important effects such as the site's capability to bind and activate CO2, competing reaction paths via intermediate isomer formation, and the role of water. Our research shows that these aspects are crucial for CO2 reduction.
JOURNAL OF CATALYSIS
(2023)
Review
Chemistry, Inorganic & Nuclear
Hussein A. Younus, Nazir Ahmad, Wenpeng Ni, Xiwen Wang, Mohammed Al-Abri, Yan Zhang, Francis Verpoort, Shiguo Zhang
Summary: Transforming wastes or hazardous materials into value-added chemical products is important for economic, environmental, and sustainable purposes. Among various approaches, electrochemical reduction of CO2 is considered the most promising method with its advantages and the increasing availability of renewable electricity sources. Molecular catalysts, particularly pincer-based molecular catalysts, have shown significant potential for controlling and designing reaction sites to better understand catalytic reaction pathways. This review focuses on the application of pincer-type complexes in CO2 reduction reaction (CO2RR), discussing reaction mechanisms, reactive intermediates, deactivation pathways, product selectivity, and stability issues of these catalysts. The insights gained from these studies can drive the development of catalysts with high selectivity and stability for efficient CO2RR, contributing to global scientific and technological prosperity.
COORDINATION CHEMISTRY REVIEWS
(2023)
Article
Chemistry, Physical
Tian-Wen Jiang, Ya-Wei Zhou, Xian-Yin Ma, Xianxian Qin, Hong Li, Chen Ding, Bei Jiang, Kun Jiang, Wen-Bin Cai
Summary: The study investigates the mechanism of CO2RR on Pd and Pd-B film electrodes using various analytical techniques, demonstrating the role of surface CO and the influence of B-doping on CO2RR at different potentials.
Review
Chemistry, Multidisciplinary
Zheng Zhang, Xin Huang, Zhou Chen, Junjiang Zhu, Balazs Endrodi, Csaba Janaky, Dehui Deng
Summary: Electrocatalytic CO2 reduction reaction (CO2RR) in membrane electrode assembly (MEA) systems is a promising technology due to the direct transport of gaseous CO2 to the cathode catalyst layer and the absence of liquid electrolyte between the cathode and the anode. Recent progress has shown the way to achieve industrially relevant performance. This review focuses on the principles of CO2RR in MEA, particularly the gas diffusion electrodes and ion exchange membranes, as well as the anode processes and voltage distribution. The generation of different reduced products and corresponding catalysts is summarized, and the challenges and opportunities for future research are highlighted.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Changlong Xiao, Jie Zhang
Summary: Electrochemical conversion of CO2 to value-added chemicals and fuels using Cu catalysts has shown promising potential, but poor product selectivity remains a major technical challenge for global applications. Tailoring the electrocatalyst architecture through nanotechnology principles can significantly impact the adsorption energetics of key intermediates and reaction pathways.
Review
Chemistry, Physical
Hassan Ait Ahsaine, Mohamed Zbair, Amal BaQais, Madjid Arab
Summary: This review explores different electrocatalysts for electrochemical CO2 reduction reactions and summarizes the requirements for the design of stable electroactive materials.
Article
Chemistry, Physical
Libo Sun, Vikas Reddu, Tan Su, Xinqi Chen, Tian Wu, Wei Dai, Adrian C. Fisher, Xin Wang
Summary: Decorating carbon nanotubes with pyridine-based functional groups can enhance the activity of molecular catalysts towards CO2 reduction. Density functional theory calculations were conducted to support the experimental findings.
Article
Chemistry, Physical
Cedric David Koolen, Wen Luo, Andreas Zuettel
Summary: This Review summarizes three decades of research on CO2RR and categorizes various metal catalysts into four size regimes. The effects of different structural factors on the catalysts in each size regime are discussed. Future directions for better understanding and further development of active and selective catalysts for CO2RR are provided.
Article
Chemistry, Physical
Minmin Wang, Min Li, Yunqi Liu, Chao Zhang, Yuan Pan
Summary: This article systematically summarizes the current research status of metal single-atomic site catalysts (SASCs) for the efficient catalysis of CO2RR, discusses various methods for enhancing the activity and selectivity of SASCs, and reviews the application of in-situ characterization technologies in SASC-catalyzed CO2RR. The article also discusses the unresolved challenges in this field and proposes future research directions for the design and application of SASCs for CO2RR.
Review
Materials Science, Multidisciplinary
Xiaojiao Li, Xiaohu Yu, Qi Yu
Summary: This article reviews the recent progress of Cu-based single-atom catalysts (SACs) in CO2 reduction reaction (CO2 RR), discussing the regulatory strategies for the interaction of the active site with key reaction intermediates. Different design strategies, including the regulation of metal centers, Cu-based single-atom alloy catalysts (SAAs), non-metal SACs, tandem catalysts, and composite catalysts, are also reviewed. Furthermore, the current challenges and future developments of SACs in CO2 RR are summarized.
SCIENCE CHINA-MATERIALS
(2023)
Review
Chemistry, Physical
Yadong Du, Xiangtong Meng, Zhen Wang, Xin Zhao, Jieshan Qiu
Summary: This article reviews recent progress in graphene-based electrocatalysts for electrocatalytic CO2 reduction (ECR). The fundamentals and evaluation parameters of ECR, as well as the methods for making graphene-based catalysts for ECR, are introduced and discussed. The relationships between graphene structures, surface functional groups, heteroatom doping configurations, metal single-atom species, surface/interface properties, and catalytic performance are highlighted. Finally, the opportunities and perspectives of graphene-based catalysts for ECR are outlined.
ACTA PHYSICO-CHIMICA SINICA
(2022)
Article
Chemistry, Multidisciplinary
Yaxi Ding, Siwen Zhang, Jiazhuo Li, Ying Sun, Bosi Yin, Hui Li, Yue Ma, Zhiqiao Wang, Hao Ge, Dawei Su, Tianyi Ma
Summary: This study demonstrates the design of a high-performance cathode for aqueous magnesium ion energy storage by doping Al3+ cations into α-MnO2 materials. The introduction of Al3+ cations adjusts the local chemical environment and precisely regulates the diffusion behavior of inserted Mg2+ cations. The enhanced elastic migration of Mg2+ cations driven by strengthened electrostatic attraction leads to lower diffusion energy barrier, improved reaction kinetics, and adaptive volume expansion.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Jichi Liu, Chongchong Wu, Ian D. Gates, Baohua Jia, Zihang Huang, Tianyi Ma
Summary: Aqueous supercapacitors are considered promising for commercial energy storage devices due to their safety, low cost, and environmental friendliness. However, the challenge of achieving both long electrode lifespan and qualified energy-storage property has hindered their practical application. In this study, an electrode-electrolyte integrated optimization strategy is developed to meet real-life device requirements. By optimizing the nanomorphology and surface chemistry of the tungsten oxide anode, along with the design of a hybrid electrolyte, record-breaking durability and stable operation under extreme conditions are achieved. These results demonstrate the possibility of replacing commercial organic energy storage devices with aqueous counterparts for various daily applications.
ENERGY & ENVIRONMENTAL 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
Yi Zhong, Chenglin Wu, Xiaofang Jia, Sijia Sun, Daimei Chen, Wenqing Yao, Hao Ding, Junying Zhang, Tianyi Ma
Summary: A Mo-doping BiVO4/ultrathin-CoAl-LDH (Mo:BVO/CoAl-LDH-u) photoanode with self-healing property is designed by using atomic layer CoAl-LDH as cocatalyst to modify Mo:BVO through dipping coating. The Mo:BVO/CoAl-LDH-u photoanode exhibits excellent surface charge separation efficiency and photocurrent density of 5.8 mA/cm2 without scavengers. CoAl-LDH-u enhances surface charge transfer efficiency and promotes the oxygen evolution reaction rate in Mo:BiVO4, while the self-healing property of Mo:BVO/CoAl-LDH-u allows for natural restoration of photoelectrochemical performance. This work provides a facile approach for fabricating high-efficiency BiVO4 photoelectrodes for PEC water splitting.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Nanoscience & Nanotechnology
Ge Yan, Xiaodong Sun, Yu Zhang, Hui Li, Hongwei Huang, Baohua Jia, Dawei Su, Tianyi Ma
Summary: A novel metal-free 2D/2D van der Waals heterojunction was successfully constructed by integrating a two-dimensional COF with ketoenamine linkage and defective hexagonal boron nitride. The presence of VDW heterojunction and introduced defects facilitated charge carriers separation and provided more reactive sites. The resulting heterojunction exhibited excellent solar energy catalytic activity for water splitting, surpassing the performance of pristine COF and other metal-free-based photocatalysts reported to date.
NANO-MICRO LETTERS
(2023)
Review
Chemistry, Physical
Chunyang Wang, Cheng Hu, Fang Chen, Tianyi Ma, Yihe Zhang, Hongwei Huang
Summary: Efficient conversion of mechanical energy via piezocatalysis has great potential in relieving energy crisis and environmental deterioration, and can be applied in sterilization, disease therapy, personal cleaning, organic synthesis, biomass conversion, and more. However, the low energy transformation efficiency hinders the practical applications of piezocatalysis, leading to the emergence of various strategies to enhance its catalytic activity. Nonetheless, selecting the proper design strategies for specific piezocatalytic applications is still challenging.
Article
Engineering, Environmental
Chengguo Li, Susumu Sato, Tianyi Ma, Kent C. Johnson, Thomas Durbin, Georgios Karavalakis
Summary: This study used portable emissions measurement systems (PEMS) to assess the on-road gaseous and particulate emissions from a gasoline direct injection (GDI) hybrid electric vehicle (HEV). Testing was conducted on three different driving routes representing urban, highway, and mountain driving conditions. Results showed that gaseous emissions were highest during mountain driving, while PM and soot emissions were comparable between urban and rural driving conditions but higher than highway driving. NOx emissions and soot emissions showed good correlation with vehicle acceleration but poor correlation with road grade.
EMISSION CONTROL SCIENCE AND TECHNOLOGY
(2023)
Article
Chemistry, Physical
Sangni Wang, Riming Hu, Ding Yuan, Lei Zhang, Chao Wu, Tianyi Ma, Wei Yan, Rui Wang, Liang Liu, Xuchuan Jiang, Hua Kun Liu, Shi Xue Dou, Yuhai Dou, Jiantie Xu
Summary: In this study, ultrathin single-atomic tungsten-doped Co3O4 nanosheets were designed and synthesized as catalytic additives in the sulfur cathode for lithium-sulfur batteries (LSBs). The tungsten-doped Co3O4 not only reduces the shuttling of lithium polysulfides but also decreases the energy barrier of sulfur redox reactions, leading to accelerated electrode kinetics. The LSB cathodes with the W-x-Co3O4 electrocatalyst exhibit high reversible capacities and excellent cycling performance.
Article
Materials Science, Multidisciplinary
Bingsen Wang, Junjun Wang, Jiaqi Li, Miao Yang, Minghao Huang, Tianyi Ma, Yu Tian, Fengmin Wu
Summary: In this study, KNNLT-BNT lead-free ceramics were prepared using the solid solution method with Mn-doped to regulate the grain size and electrical properties. The doped concentrations were 0.3%, 0.4%, and 0.5%. The surface structure and internal structure of the ceramics were characterized, showing improved compactness and lattice distortion with increasing Mn-doped concentration. The electrical properties were characterized by optical band gap and dielectric constant, and the analysis revealed that the best performance was achieved at a Mn-doped concentration of 0.5%, with a normal distribution of grain size and the narrowest band gap width of 2.693 eV.
Article
Chemistry, Physical
Suwen Wang, Chengfang Song, Yanjiang Cai, Yongfu Li, Peikun Jiang, Hui Li, Bing Yu, Tianyi Ma
Summary: MXenes are commonly considered to be catalytically inert, but a strategy of interfacial polarization is proposed to improve their catalytic activity. By constructing an interfacial structure consisting of black phosphorus (BP) nanoflakes and Nb2C MXene nanosheets, the catalytic performance of MXenes is enhanced for electrochemical nitrate reduction to ammonia. The strong interfacial polarization between BP nanoflakes and Nb2C nanosheets in the prepared BP/Nb2C composite leads to the formation of positively centered Nb atoms and BP-polarized Nb atoms, which synergistically catalyze the cleavage of N-O bonds in HNO2* to form NO*. The stabilization of monatomic *N by the BP/Nb2C composite is also improved. The ammonia yield rate and Faraday efficiency of the BP/Nb2C composite are significantly higher compared to BP nanoflakes and Nb2C nanosheets.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Kailai Zhang, Xiaodong Sun, Haijun Hu, Ge Yan, Anqi Qin, Yali Ma, Hongwei Huang, Tianyi Ma
Summary: Defect engineering is used to optimize the piezocatalytic performance of microcrystalline cellulose (MCC), improving its electrical conductivity and the separation and transfer efficiency of piezoelectric charges. The piezocatalytic H-2 production rate of MCC with the optimal defect concentration reaches 84.47 mu mol g(-1) h(-1) under ultrasonic vibration, approximately 3.74 times higher than pure MCC. Moreover, MCC with the optimal defect concentration achieves a commendable piezocatalytic H-2 production rate of 93.61 mu mol g(-1) h(-1) in natural seawater.
Article
Chemistry, Inorganic & Nuclear
Haijun Hu, Xiaodong Sun, Kailai Zhang, Yang Chen, Hui Li, Hongwei Huang, Yali Ma, Tianyi Ma
Summary: Photocatalytic water splitting using a semiconductor is an effective way to obtain clean energy. However, pure semiconductors have poor photocatalytic performance due to charge carrier recombination, limited light harvesting ability and deficiency of surface reactive sites. In this study, a new UiO-66-NH2/CdIn2S4 (NU66/CIS) heterojunction nanocomposite was synthesized using the hydrothermal method, which showed improved performance in water reduction. The NU66/CIS heterojunction had intimate connections and promoted effective transfer of electrons, resulting in enhanced H-2 production. This research offers a creative idea for constructing active MOF-based photocatalysts for H-2 evolution.
DALTON TRANSACTIONS
(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)
