Review
Chemistry, Multidisciplinary
Xinning Song, Liang Xu, Xiaofu Sun, Buxing Han
Summary: Utilizing CO2 for producing fuels and chemicals has advantages of abundance, non-toxicity, and economy. However, the complex reaction process of multi-electronic products makes it challenging to achieve high selectivity, current density, overpotential, and stability simultaneously. In situ/operando characterization techniques have played an important role in understanding the reaction pathway of CO2RR. This mini-review discusses recent progress on in situ/operando characterizations, including microscopy, infrared spectroscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, and X-ray absorption fine spectroscopy, and addresses the capabilities and challenges of these techniques.
SCIENCE CHINA-CHEMISTRY
(2023)
Review
Materials Science, Multidisciplinary
Yanzheng He, Sisi Liu, Mengfan Wang, Qiyang Cheng, Haoqing Ji, Tao Qian, Chenglin Yan
Summary: Gas-involved electrochemical reactions offer viable solutions to the global energy crisis and environmental pollution. In situ techniques have gained significant attention as judicious tools for real-time monitoring of the variations in catalysts, intermediates, and products during the reaction process, providing insights into reaction mechanisms, material structures, and active sites. This review highlights the recent progress of various advanced in situ characterization techniques, such as in situ X-ray based technologies, in situ spectrum technologies, and in situ scanning probe technologies, in enhancing our understanding of heterogeneous electrocatalytic reactions. The development and applications of these techniques, along with key questions that need to be addressed, are summarized.
ENERGY & ENVIRONMENTAL MATERIALS
(2023)
Article
Chemistry, Physical
Shahid Zaman, Shenghua Chen
Summary: This study discusses the inaccuracies and differences in evaluating techniques for the oxygen reduction reaction (ORR) and carbon dioxide reduction reaction (CO2RR), leading to difficulties in comparing and validating the activity of catalysts. The study suggests the need for standardized methods and protocols to measure ORR and CO2RR performance.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Physical
Bishnubasu Giri, Arup Mahata, Tatinaidu Kella, Debaprasad Shee, Filippo De Angelis, Somnath Maji
Summary: The introduction of tetrazole moiety into the ligand framework of isomeric ruthenium catalysts has altered the catalytic pathway for the electrochemical reduction of CO2 to CO, resulting in significantly lower over-potential and the formation of a metallocarboxylate intermediate. The mechanism follows the ECE pathway and has been supported by various characterization techniques and theoretical studies.
JOURNAL OF CATALYSIS
(2022)
Article
Electrochemistry
Lingmei Ni, Pascal Theis, Stephen Paul, Robert W. Stark, Ulrike Kramm
Summary: This study reports on an in situ Mossbauer spectroelectrochemical study of a porphyrin-based catalyst for the oxygen reduction reaction (ORR) in fuel cells. By comparing to in situ Fe-57 Mossbauer spectra, the contributions to different ORR pathways can be identified and associated with iron signatures, enabling the determination of mass-based site density and turn-over frequency data for relevant conditions. This work sheds light on the mechanism of the oxygen reduction reaction involved in FeNC catalysts.
ELECTROCHIMICA ACTA
(2021)
Review
Chemistry, Multidisciplinary
Janis Timoshenko, Beatriz Roldan Cuenya
Summary: X-ray absorption spectroscopy (XAS) is a crucial method for investigating the structure and composition of heterogeneous catalysts, revealing the nature of active sites and establishing links between structural motifs, local electronic structure, and catalytic properties. Recent advancements in instrumentation and data analysis approaches for deciphering X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectra have been discussed, with emphasis on applications in the field of heterogeneous catalysis, particularly in electrocatalysis.
Review
Chemistry, Multidisciplinary
Bin Wu, Haibing Meng, Dulce M. Morales, Feng Zeng, Junjiang Zhu, Bao Wang, Marcel Risch, Zhichuan J. Xu, Tristan Petit
Summary: Nitrogen-doped carbons are a rapidly growing class of materials for oxygen electrocatalysis, offering low cost, environmental friendliness, excellent conductivity, and scalable synthesis. They have the potential to replace precious metal-based electrocatalysts and reduce costs in energy conversion and storage systems.
ADVANCED FUNCTIONAL MATERIALS
(2022)
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)
Article
Chemistry, Physical
Yinlong Jiang, Qingsong Chen, Di Wang, Xin Li, Yuping Xu, Guocong Guo
Summary: Bismuth-based catalysts have been extensively studied for electrocatalytic CO2 reduction to formate. Most studies focus on activity, selectivity, and durability, neglecting the stability of catalysts' structure during CO2 electrolysis. This research investigates the structural evolution of bismuth-based catalysts under different electrolytes and reveals their performance variations. The results provide valuable insights for the design and synthesis of efficient catalysts for CO2 electroreduction.
Article
Chemistry, Multidisciplinary
Qi Zhao, Chao Zhang, Riming Hu, Zhiguo Du, Jianan Gu, Yanglansen Cui, Xiao Chen, Wenjie Xu, Zongju Cheng, Songmei Li, Bin Li, Yuefeng Liu, Weihua Chen, Chuntai Liu, Jiaxiang Shang, Li Song, Shubin Yang
Summary: An efficient method for producing single atom copper immobilized MXene for catalyzing CO2 reduction to methanol through selective etching of hybrid A layers in quaternary MAX phases was demonstrated. The single atom Cu catalyst exhibited high Faradaic efficiency and good electrocatalytic stability, attributed to its unique electronic structure and surface functional groups.
Article
Chemistry, Physical
Haidong Shen, Yike Zhao, Ling Zhang, Yuan He, Shaowei Yang, Tianshuai Wang, Yueling Cao, Ying Guo, Qiuyu Zhang, Hepeng Zhang
Summary: A CuS-Bi2S3 heterojunction precursor that can in situ reconstruct to Cu-doped Bismuth (CDB) electrocatalyst during CO2RR is reported. The CDB exhibits high CO2RR performance with industrial-compatible current density and formate formation rate.
ADVANCED ENERGY MATERIALS
(2023)
Review
Chemistry, Physical
Huimin Wang, Jingjing Huang, Jinmeng Cai, Yingying Wei, Ang Cao, Baozhong Liu, Siyu Lu
Summary: With the development of industrial and agricultural activities, the excessive production of nitrate has become a serious environmental and public health concern. Among various nitrate treatment techniques, electrochemical nitrate reduction reaction (eNRR) has gained significant attention due to its mild conditions and pollution-free nature. However, understanding the eNRR mechanism requires the use of in situ and operando techniques to study the reaction process at a time-resolved and atomic level.
Article
Chemistry, Multidisciplinary
Jieyi Shen, Lishuang Wang, Xuedong He, Shun Wang, Jiadong Chen, Juan Wang, Huile Jin
Summary: In this study, a new class of Cu/In2O3 nanoparticles was prepared as superior electrocatalysts for CO2RR, which exhibited high CO/H-2 ratios and total faradaic efficiency in a wide potential range. The excellent performance of these catalysts was attributed to the electronic interaction between amorphous In2O3 and Cu, expanding the possibilities for designing and preparing fascinating electrocatalysts for CO2RR.
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, Physical
Liliana P. L. Gonsalves, Jerrik Mielby, O. Salome G. P. Soares, Juliana P. S. Sousa, Dmitri Y. Petrovykh, Oleg I. Lebedev, M. Fernando R. Pereira, Soren Kegnaes, Yury V. Kolen'ko
Summary: Understanding the reaction mechanism on different materials can optimize the development of cost-efficient, high-performing catalysts for CO2 methanation at low temperatures. Ni nanoparticles supported on a carbon/CeO2 composite and pure CeO2 show excellent low-temperature activity, achieving up to 87% CO2 conversion with full selectivity towards CH4 at 370 degrees C. The study of the reaction mechanism reveals that the CO2 methanation reaction follows a combination of the CO and formate pathways on pure CeO2, while it only follows the formate pathway on the carbon/CeO2 composite.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Engineering, Electrical & Electronic
Kang Jea Lee, Duc Anh Dinh, Huynh Tran My Hoa, Pham Hoai Phuong, Hoang Hung Nguyen, Kwan San Hui, Kwun Nam Hui, Tran Viet Cuong
Summary: In this study, plasmonic coupling effect was utilized to enhance the whispering gallery mode (WGM) resonance emission in InGaN/GaN multi-quantum well (MQW) microdisks by decorating Ag nanoparticles on microdisks.
JOURNAL OF ELECTRONIC MATERIALS
(2022)
Article
Chemistry, Physical
Yao Kang, Shuo Wang, Kwan San Hui, Shuxing Wu, Duc Anh Dinh, Xi Fan, Feng Bin, Fuming Chen, Jianxin Geng, Weng-Chon Max Cheong, Kwun Nam Hui
Summary: This study presents a simple method to activate surface reconstruction on Ni(OH)(2) by incorporating F anions, leading to enhanced oxygen evolution reaction (OER) activity. Experimental results show that the incorporation of F ions facilitates surface reconstruction and the transformation of Ni(OH)(2) into a mesoporous and amorphous F-NiOOH layer.
Article
Chemistry, Physical
Yuwei Zhao, Donghai Wu, Tingting Tang, Chongguang Lyu, Junfeng Li, Shunping Ji, Cheng-zong Yuan, Kwan San Hui, Chenyang Zha, Kwun Nam Hui, Houyang Chen
Summary: This article introduces an in situ tailored interface strategy for removing capping agents from the surface of copper sulfide and enhancing its catalytic activity. The method allows for the production of clean copper sulfide surfaces without the need for harsh processing conditions or non-commercial materials, leading to improved battery performance.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Physical
Bari Wulan, Lanling Zhao, Dongxing Tan, Xueying Cao, Jizhen Ma, Jintao Zhang
Summary: It has been demonstrated that the electrochemical transformation of bismuth sulfide nanorods can lead to the formation of a three-dimensional bismuth nanosheet network on functionalized carbon fibers, improving the performance of the carbon dioxide reduction reaction. The hierarchical bismuth nanosheet network shows high selectivity, large current density, and good long-term stability.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Applied
Xinxin Shu, Maomao Yang, Miaomiao Liu, Wei Pan, Jintao Zhang
Summary: The coordination structure of cobalt with nitrogen atoms on reduced graphene oxide (rGO) sheets was successfully regulated by a bridging strategy involving interfacial complexation and thermal treatment. The well-dispersed cobalt-nitrogen coordination structure on rGO enables efficient oxygen reduction and evolution reactions, leading to the excellent performance of the fabricated Zn-air battery in terms of power density and long-term stability.
JOURNAL OF ENERGY CHEMISTRY
(2022)
Article
Chemistry, Physical
Haixing Gao, Shuo Wang, Weng-Chon (Max) Cheong, Kaixi Wang, Huifang Xu, Aijian Huang, Junguo Ma, Jiazhan Li, Weng-Fai (Andy) Ip, Kwan San Hui, Duc Anh Dinh, Xi Fan, Feng Bin, Fuming Chen, Kwun Nam Hui
Summary: Ultrathin nitrogen-doped carbon nanosheets with intrinsic defects were synthesized through the pyrolysis of ZIF-8 with linker vacancies. The as-synthesized electrocatalyst exhibited excellent oxygen reduction reaction (ORR) activity and zinc-air battery performance. The adjacent sp3-carbon was found to enhance the adsorption and activation of oxygen molecules on sp2-carbon, leading to a lower ORR overpotential.
Article
Chemistry, Multidisciplinary
Kaixi Wang, Shuo Wang, Kwan San Hui, Junfeng Li, Chenyang Zha, Duc Anh Dinh, Zongping Shao, Bo Yan, Zikang Tang, Kwun Nam Hui
Summary: A 3D quasi-parallel structure consisting of dense Pt nanoparticles immobilized on oxygen vacancy-rich NiOx heterojunctions has been developed as an alkaline hydrogen evolution reaction (HER) catalyst. The catalyst exhibits extraordinary HER performance with a low overpotential, high mass activity, and long durability. When combined with NiFe-layered double hydroxide, the assembled alkaline electrolyzer requires extremely low voltage and can operate stably for a long time.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Cheng-Zong Yuan, Shuo Wang, Kwan San Hui, Kaixi Wang, Junfeng Li, Haixing Gao, Chenyang Zha, Xiaomeng Zhang, Duc Anh Dinh, Xi-Lin Wu, Zikang Tang, Jiawei Wan, Zongping Shao, Kwun Nam Hui
Summary: The synergistic regulation of the electronic structures of transition-metal oxide-based catalysts via oxygen vacancy defects and single-atom doping is efficient to boost their oxygen evolution reaction (OER) performance. In this study, a facile defect-induced in situ single-atom deposition strategy is developed to anchor atomically dispersed Ru single-atom onto oxygen vacancy-rich cobalt oxides (Ru/Co3O4-x) based on the spontaneous redox reaction between Ru3+ ions and nonstoichiometric Co3O4-x. The as-prepared Ru/Co3O4-x electrocatalyst with the coexistence of oxygen vacancies and Ru atoms exhibits excellent performances toward OER.
Article
Chemistry, Physical
Shunping Ji, Yunshan Zheng, Kwan San Hui, Junfeng Li, Kaixi Wang, Chunyan Song, Huifang Xu, Shuo Wang, Chenyang Zha, Duc Anh Dinh, Zikang Tang, Zongping Shao, Kwun Nam Hui
Summary: By mixing amorphous zinc phosphate with black phosphorus nanomaterials, the agglomeration of black phosphorus can be weakened, and the volume expansion can be reduced, thus improving the stability of the composite electrode in humid air. The optimized amorphous black phosphorus/zinc phosphate composite anode retains a capacity of 369.0 mA h g-1 and reduces the volume expansion to 47% compared to the untreated electrode. Additionally, the amorphous zinc phosphate can absorb water, resulting in good environmental stability even after exposure to humid air for two days, with a reversible capacity of 629.2 mA h g-1.
ENERGY STORAGE MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yunshan Zheng, Junfeng Li, Shunping Ji, Kwan San Hui, Shuo Wang, Huifang Xu, Kaixi Wang, Duc Anh Dinh, Chenyang Zha, Zongping Shao, Kwun Nam Hui
Summary: In this study, a Zn-doped K0.02Na0.55Mn0.70Ni0.25Zn0.05O2 material (denoted as KNMNO-Z) was reported to inhibit the Jahn-Teller effect and reduce the irreversible phase transition in potassium-ion batteries. Through the Zn-doping strategy, higher Mn valence was achieved, leading to an improvement in cyclic stability with a high retention rate of 97% after 1000 cycles.
Article
Chemistry, Multidisciplinary
Jiawu Peng, Xiaoting Hong, Qiongxiang Zhou, Kwan San Hui, Bin Chen
Summary: This study presents a method for synthesizing microspherical FePO4·2H2O precursors with secondary nanostructures by the electroflocculation of low-cost iron fillers in a hot solution. The effect of precursor structure and morphology on the electrochemical performance of the synthesized LiFePO4/C was investigated. The improved performance of LiFePO4/C was attributed to the enhanced Li+ diffusion rate and the crystallinity of LiFePO4/C.
Article
Chemistry, Multidisciplinary
Zhenjiang Yu, Hongmei Shan, Yunlei Zhong, Guo Hong, Kwan San Hui, Xia Zhang, Kwun Nam Hui
Summary: This study presents a lithium-free V2O5 cathode for application in polymer-based solid-state batteries (SSBs) with high energy density. The microstructured transport channels and suitable operational voltage enable the utilization of polymer-based solid-state electrolyte (SSE). The V2O5 cathode, constructed through microstructural engineering, exhibits improved electrochemical performance and cycling stability in SSBs.
Article
Chemistry, Physical
Shuo Wang, Lei Li, Kwan San Hui, Duc Anh Dinh, Zhiyi Lu, Qiuju Zhang, Kwun Nam Hui
Summary: Electrochemical nitrate reduction reaction (NO3RR) has potential in wastewater management and carbon-neutral ammonia synthesis, but lacks high-quality catalysts with controllable reaction pathways and high activity and selectivity. In this study, we explore the application of single atom alloys (SAAs) in nitrate reduction through high-throughput first-principles calculations. We identify Ni/Cu(111) as the most active SAA catalyst for NO3RR and find that the adsorption free energy of *NO3 can serve as an efficient descriptor to design and predict the NO3RR performance of SAAs. Furthermore, we reveal the pH-dependent properties of Cu-based SAAs, which influence the competition between the hydrogen evolution reaction (HER) and NO3RR.
Article
Chemistry, Physical
Junfeng Li, Yunshan Zheng, Kwan San Hui, Kaixi Wang, Chenyang Zha, Duc Anh Dinh, Jiguo Tu, Zongping Shao, Kwun Nam Hui
Summary: A carbothermal reduction approach and stable electrode/electrolyte interface construction regulated by voltage are used to ensure the ultra-long cycling performance of potassium ion batteries (PIBs) with pure-phase KVOPO4 materials. The KVOPO4 materials demonstrate a stable 3D crystal framework and efficient K+ diffusion, leading to high reversibility and low-capacity decay upon cycling. The exceptional structure and robust electrode/electrolyte interface of KVOPO4 materials explain their cycling stability.
ENERGY STORAGE MATERIALS
(2023)
Article
Chemistry, Physical
Cheng-Zong Yuan, Shuo Wang, Kwan San Hui, Kaixi Wang, Junfeng Li, Haixing Gao, Chenyang Zha, Xiaomeng Zhang, Duc Anh Dinh, Xi-Lin Wu, Zikang Tang, Jiawei Wan, Zongping Shao, Kwun Nam Hui
Summary: The synergistic regulation of electronic structures of transition-metal oxide-based catalysts using oxygen vacancy defects and single atom doping can significantly enhance their performance in oxygen evolution reaction (OER). In this study, a simple defect-induced in situ single-atom deposition strategy was developed to deposit atomically dispersed Ru single atoms onto oxygen vacancy-rich cobalt oxides (Ru/Co3O4-x) by a spontaneous redox reaction. The resulting Ru/Co3O4-x electrocatalyst, with the coexistence of oxygen vacancies and Ru atoms, exhibited excellent OER performance with a low overpotential, small Tafel slope value, and good long-term stability in alkaline media. Density functional theory calculations revealed that the synergy between oxygen vacancies and atomically dispersed Ru can optimize the adsorption of oxygen-based intermediates and reduce the reaction barriers of OER by tailoring the electron decentralization and d-band center of Co atoms. This study proposes a feasible strategy for constructing electrocatalysts with abundant oxygen vacancies and atomically dispersed noble metals, and provides a deep understanding of the electronic engineering of transition-metal-based catalysts to boost OER.
