Review
Chemistry, Physical
Ziheng Zhan, Zhiyi Sun, Zihao Wei, Yaqiong Li, Wenxing Chen, Shenghua Li, Siping Pang
Summary: Rare earth elements play a crucial role in optimizing catalyst performance in energy conversion processes through their unique electronic and orbital structures. This review focuses on the atomic interface regulation role of rare earth elements, using atomic level doped rare earth elements as an example, and summarizes their regulatory mechanisms in various energy conversion applications.
Review
Materials Science, Multidisciplinary
Yingping Pang, Chao Su, Liqiang Xu, Zongping Shao
Summary: Photocatalytic or electrocatalytic transformation of N-2-to-NH3 offers potential for sustainable agricultural production and portable carbon-free energy carrier. Single-atom catalysts (SACs) have emerged as promising candidates for NH3 photo/electrosynthesis due to their high activity, selectivity, and stability. This article provides an overview of recent advances in this research area, including fundamental understanding, synthesis strategies, analytical techniques, and theoretical simulations. The challenges in N-2 reduction and the state-of-the-art SACs as photo/electrocatalysts for NH3 production are also discussed.
PROGRESS IN MATERIALS SCIENCE
(2023)
Review
Chemistry, Multidisciplinary
Yujing Ren, Jinyong Wang, Mingyue Zhang, Yuqing Wang, Yuan Cao, Dong Ha Kim, Zhiqun Lin
Summary: Single-atom catalysts face limitations in their practical applications, but arranging randomly dispersed single atoms into locally ordered single-atom catalysts (LO-SACs) can greatly enhance their performance and simplify reaction mechanisms. This review comprehensively introduces the characteristics, synthetic strategies, characterization methods, and applications of LO-SACs in electrocatalysis, as well as the future opportunities and challenges.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Xinjiang Hu, Daixi Zhou, Hui Wang, Wenlong Zhang, Haoxiang Zhong, Yongsheng Chen
Summary: Single atom catalysts (SACs) based on M1-Nx-Cy have emerged as a frontier research field in catalysis, offering high reactivity, maximum atomic utilization, and high selectivity. This review summarizes the fabrication methods of M1-Nx-Cy based SACs via support anchoring and coordination design strategies, characterizes single metal atoms, and discusses their environmental applications. The potential of M1-Nx-Cy based SACs to address current and future environmental pollution problems is emphasized.
CHINESE CHEMICAL LETTERS
(2023)
Review
Chemistry, Applied
Xiaolong Tang, Feng Li, Fang Li, Yanbin Jiang, Changlin Yu
Summary: Hydrogen peroxide (H2O2) is widely used as an environmentally friendly oxidant and the production via the photocatalytic and electrocatalytic methods using single-atom catalysts (SACs) has advantages of simple and controllable conditions and non-polluting reaction products. The review discusses the mechanisms and advantages of SACs, presents recent progress in H2O2 production, and explores future directions for SACs in photocatalytic and electrocatalytic H2O2 production.
CHINESE JOURNAL OF CATALYSIS
(2023)
Review
Chemistry, Multidisciplinary
Wenxin Guo, Zhiyuan Wang, Xiaoqian Wang, Yuen Wu
Summary: Single-atom catalysts (SACs) are a promising new material with excellent activity, selectivity, and stability, making them ideal for various important reactions. The precise synthesis of SACs, including the control of coordination structure and choice of different systems, is crucial for their application in different fields. However, challenges in large-scale preparation and industrialization still need to be addressed for the rapid development of SACs.
ADVANCED MATERIALS
(2021)
Review
Chemistry, Applied
Rongchen Shen, Lei Hao, Yun Hau Ng, Peng Zhang, Arramel Arramel, Youji Li, Xin Li
Summary: This review focuses on the intrinsic electronic structure, catalytic mechanism, and activity of metal-nitrogen-based single-atom catalysts (SACs) in photocatalysis and electrocatalysis. By analyzing the fundamentals of M-N-based SACs and combining theoretical calculations and experimental investigations, a comprehensive understanding of the improved coordination structure and observed activity is provided. Lastly, the challenges and prospects for constructing highly active M-N-based photocatalysis and electrocatalysis SACs are discussed.
CHINESE JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Jiapeng Ji, Lei Wu, Shiyu Zhou, Tong Qiu, Zeheng Li, Liguang Wang, Liang Zhang, Lu Ma, Min Ling, Shaodong Zhou, Chengdu Liang
Summary: The electronic structure of single-atom catalysts (SACS) plays a critical role in bifunctional oxygen electrocatalysis. In this study, the electronic structure was effectively adjusted by introducing a heterogenous metal that bonded directly to the active center atom. This adjustment resulted in optimized binding energy and reduced energy barriers for catalytic reactions. Theoretical calculations confirmed these effects and the uniform distribution of 3d orbitals, which improved the bifunctional oxygen electrocatalytic reactivity. The constructed bifunctional catalyst exhibited outstanding electrocatalytic performances in various energy storage systems. The generality and expandability of this strategy were demonstrated by the successful development of other dual-metal catalysts systems with different active metals.
Review
Nanoscience & Nanotechnology
Qin Zhang, Xiaoxiang Zhang, Junzhong Wang, Congwei Wang
Summary: Supported metal nanostructures are widely studied heterogeneous catalysts, with isolated metal atoms maximizing activity. Graphene-supported SACs offer great potential as efficient electrocatalysts, but challenges remain for further improvement.
Article
Chemistry, Multidisciplinary
Chenghong Hu, Yajing Wang, Jianmin Chen, Hao-Fan Wang, Kui Shen, Kewen Tang, Liyu Chen, Yingwei Li
Summary: In this study, the authors demonstrate that introducing HER-inert main-group metal single atoms adjacent to transition-metal single atoms can enhance the CO2RR to CO without inducing the HER side reaction. The dual-metal Cu and In single-site atoms prepared by pyrolysis show superior catalytic performance compared to their monometallic counterparts.
Article
Chemistry, Multidisciplinary
Ruisong Li, Wenjun Fan, Peng Rao, Junming Luo, Jing Li, Peilin Deng, Daoxiong Wu, Wei Huang, Chunman Jia, Zhongxin Liu, Zhengpei Miao, Xinlong Tian
Summary: This study successfully synthesized multimetallic single-atom catalysts (MM-SACs) using metal-C(3)N(4) and nitrogen-doped carbon as cornerstones, and verified their atomic dispersion and strong electronic reciprocity between multimetallic sites. It was found that FeCoZn-SACs and FeCoCuZn-SACs exhibited superior oxygen evolution reaction and oxygen reduction reaction activity, as well as outstanding bifunctional durability. The Co sites in FeCoCuZn-SACs were crucial contributors to the efficient catalysis of both ORR and OER. Furthermore, Zn-air batteries with FeCoCuZn-SACs as cathodic catalysts showed high power density, specific capacity, and stability for charging-discharging processes.
Review
Chemistry, Multidisciplinary
Chuang Fan, Wenrou Dong, Yousaf Saira, Yawen Tang, Gengtao Fu, Jong-Min Lee
Summary: Metal-organic frameworks (MOFs) and their derivatives, integrated with rare earth (RE) elements, have shown remarkable potential in the field of photo/electrocatalysis. The incorporation of RE can effectively enhance the catalytic performance of MOFs by regulating their electronic structure and coordination environment. This review provides a comprehensive summary and discussion of the progress and applications of RE-modified MOFs and their derivatives in photo/electrocatalysis, as well as the challenges and prospects for further research.
Article
Chemistry, Multidisciplinary
Huicheng Hu, Wenhao Guan, Yafeng Xu, Xuchun Wang, Linzhong Wu, Min Chen, Qixuan Zhong, Yong Xu, Youyong Li, Tsun-Kong Sham, Xiaohong Zhang, Lu Wang, Muhan Cao, Qiao Zhang
Summary: The study demonstrates that Pt single atoms can be successfully deposited on CsPbBr3 NCs through a photoassisted approach, leading to efficient photocatalytic properties. CsPbBr3 nanocrystals can also be used as suitable substrates for anchoring other metal single atoms, expanding their applications in catalysis.
Review
Chemistry, Physical
Sourav Ghoshal, Atish Ghosh, Prodyut Roy, Biswajit Ball, Anup Pramanik, Pranab Sarkar
Summary: Nanoclusters, single-atom, and cluster catalysts are crucial for electrochemical and photochemical nitrogen reduction reactions, and significant progress has been made in this field.
Review
Chemistry, Multidisciplinary
Huaxing Li, Rongjie Li, Gang Liu, Maolin Zhai, Jiaguo Yu
Summary: Artificial photosynthesis aims to convert solar energy into chemical energy, mitigate environmental pollution, and produce sustainable solar fuels and chemicals. The key to artificial photosynthesis systems is efficient, robust, and low-cost photocatalysts. Single-atom catalysts (SACs) and dual-atom catalysts (DACs) have gained significant attention due to their unique photocatalytic properties, while noble-metal-free catalysts offer abundance, availability, and cost-effectiveness for scalable implementation. This review outlines the principles, synthesis methods, and recent advances in SACs and DACs based on non-noble metals, using organic or inorganic substrates as scaffolds in solar-light-driven photocatalytic reactions. The review concludes with discussing the challenges, opportunities, and future prospects of noble-metal-free SACs and DACs for artificial photosynthesis.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Shiya Wu, Wei Xiong, Hao Li
Summary: Iron-based oxides have been widely used in electrochemical sensing due to their abundant sources, excellent biocompatibility, and high catalytic activity. This study focuses on the effect of different oxidation states of iron oxide nanoparticles (Fe2O3 NPs) on the electrochemical sensing performance of heavy metal ions (HMIs). The results show that the Fe2+/Fe3+ ratio and oxygen vacancy content in Fe2O3 NPs can be tuned by changing the annealing temperature, and the electrochemical sensing performance improves with the increase in the Fe2+/Fe3+ ratio. The Fe2O3 NPs-550 electrode with optimal Fe2+/Fe3+ ratio and oxygen vacancy content exhibits the best performance for simultaneously detecting Pb2+ and Cu2+.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Chemistry, Multidisciplinary
Yu Zhu, Xuan Wang, Xiaoheng Zhu, Zixin Wu, Dongsheng Zhao, Fei Wang, Dongmei Sun, Yawen Tang, Hao Li, Gengtao Fu
Summary: This study aims to improve the oxygen evolution reaction (OER) activity of layered double-hydroxide (LDH) by doping with erbium (Er). The results demonstrate that the optimal Er-doped NiFe-LDH catalyst exhibits superior performance in terms of low overpotential, high turnover frequency, and low activation energy. Electrochemical and theoretical calculations provide insights into the enhanced OER kinetics through Er doping.
Article
Chemistry, Physical
Lecheng Liang, Meng Li, Bentian Zhang, Jinhui Liang, Binwen Zeng, Liming Wang, Yawen Tang, Gengtao Fu, Zhiming Cui
Summary: This work demonstrates a new catalyst prototype, PdFe3N, for formic acid oxidation reaction (FAOR) with ordered and isolated Pd sites. The as-synthesized PdFe3N/N-rGO shows enhanced catalytic activity, robust stability, and Fe anti-dissolution properties compared to other catalysts. The DFT calculations confirm the benefits of isolated Pd sites for high formate coverage and the suppression of CO formation/poisoning.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Meng Li, Xuan Wang, Kun Liu, Huamei Sun, Dongmei Sun, Kai Huang, Yawen Tang, Wei Xing, Hao Li, Gengtao Fu
Summary: In this work, a high-performance P-Ce SAs@CoO catalyst was designed and synthesized, and its oxygen evolution reaction (OER) mechanism and active sites were investigated through experimental and theoretical analysis. The results provide a basis for the structural design and mechanistic understanding of high-performance RE-TMO catalysts.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Zhongyuan Guo, Chuangwei Liu, Chenghua Sun, Jiang Xu, Hao Li, Tianyi Wang
Summary: Single-atom catalysts have the potential for high activity and selectivity in electrocatalytic nitrogen reduction reaction (eNRR). In this study, we found that the coordination environment of single-atom Fe plays a crucial role in determining the N-2 adsorption and activation. The concept catalysts, FeCN2 and FeCN3, showed the highest eNRR activities with suppressed side reactions. Furthermore, the Bader charge of single-atom Fe and *NH adsorption energy can serve as good descriptors for the design of eNRR catalysts. This study unravels the key role of coordination environment in tuning the reactivity of single-atom Fe-N-x-C materials in eNRR.
Article
Chemistry, Physical
Xuan Wang, Meng Li, Pu Wang, Dongmei Sun, Linfei Ding, Hao Li, Yawen Tang, Gengtao Fu
Summary: A Mott-Schottky catalyst consisting of Er2O3-Co particles implanted into carbon nanofibers (Er2O3-Co/CNF) is designed to enhance alkaline oxygen reduction reaction (ORR) via spin-selective coupling. The optimized Er2O3-Co/CNF shows improved ORR performance compared to individual Co/CNF and Er2O3/CNF. The introduction of Er2O3 optimizes the electronic structure of Co through gradient orbital coupling, resulting in significantly enhanced ORR performance. This work provides new perspectives for the design of efficient ORR electrocatalysts by engineering spin-selective coupling induced by rare-earth oxides.
Article
Materials Science, Multidisciplinary
Congxu Wu, Xiujing Xing, Wei Xiong, Hao Li
Summary: In this study, nitrogen-doped mesoporous hollow carbon nanospheres (N-MHCNs) were successfully synthesized using a Stober method. The N-MHCNs showed excellent electrochemical performance in supercapacitors, with a high specific capacitance of 241 F g-1, good rate performance (capacity retention rate of 79% when current density increases from 0.5 to 10 A g-1), and good cycling ability (capacity retention rate of 90.4% after 3000 cycles). This research provides new opportunities for the synthesis of hollow mesoporous nanospheres and has potential applications in energy storage. Overall rating: 8/10.
DIAMOND AND RELATED MATERIALS
(2023)
Article
Chemistry, Physical
Jing Li, Zhongyuan Guo, Jiacheng Wu, Zhi Zheng, Zixun Yu, Fangxin She, Leo Lai, Hao Li, Yuan Chen, Li Wei
Summary: It is demonstrated that dextran, a branched sugar widely used in eyedrop products, is a multifunctional electrolyte additive for high-performance aqueous Zn ion batteries (ZIBs). Dextran functions as a surface protective layer, facilitates [Zn(H2O)(6)](2+) desolvation, preferentially adsorbs on Zn(0002) planes, and homogenizes the electric field. ZIBs with dextran show excellent performance in terms of Coulombic efficiency, plating capacity, cycle stability, and mechanical flexibility.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Congxu Wu, Wei Xiong, Hao Li
Summary: Hierarchically porous carbon foam composites with highly dispersed Fe2O3 nanoparticles were fabricated through hydrolysis-driven emulsion polymerization strategy. The resulting carbon-based composite materials containing iron oxides showed the largest specific surface area (549 m(2)/g) and pore volume (0.46 cm(3)/g). The electrode of HCF@Fe2O3 NPs-2 exhibited good capacitive properties, including high specific capacitance (225 F/g at 0.2 A/g current density) and excellent magnification performance (80% capacity retention rate as current density increased from 0.2 to 10 A/g). Moreover, HCF@SnO2 NPs was successfully synthesized by replacing hydrolyzed tin tetrachloride with ferric chloride. This study provides a new idea for the preparation of metal oxide-carbon matrix composites and highlights the potential of carbon foams in energy storage applications.
Article
Chemistry, Multidisciplinary
Heng Liu, Di Zhang, Stuart M. Holmes, Carmine D'Agostino, Hao Li
Summary: The anion exchange membrane fuel cell (AEMFC) offers a promising way for the broad application of earth-abundant element based catalysts in alkaline media. Recent studies found that zirconium nitride (ZrN) exhibits superior activity in the alkaline oxygen reduction reaction (ORR), even surpassing that of Pt. This study proposes a new theoretical framework to understand the ORR mechanism of ZrN and applies it to other transition metal nitrites. The findings provide insights for the rational design of transition metal nitrides for alkaline ORR.
Article
Chemistry, Physical
Minghu Zhao, Yuefeng Zhang, Ruijie Yang, Chen Wang, Chao Xiong, Hao Li, Rongshu Zhu, Shixing Wang, Zhiyuan Zeng
Summary: In this study, a magnetic sulfur-doped composite CoFe2O4@S-CoWO4 (CF@S-CoWO4) was developed and used for the selective recovery of gold in aqueous media. The CF@S-CoWO4 exhibited superior adsorption capacity and selectivity for gold ions compared to other materials. The composite also showed good reusability and demonstrated potential for the recycling of gold ions from electronic wastewater.
Article
Chemistry, Physical
Chuangwei Liu, Haoren Zheng, Tianyi Wang, Xiaoli Zhang, Zhongyuan Guo, Hao Li
Summary: Asymmetrical silicon-metal dimer catalysts (SiM@C3N4) were designed for electrocatalytic nitrogen reduction reaction. SiMo@C3N4 and SiRu@C3N4 showed the highest activities and suppressed the competing hydrogen evolution reaction. This research provides a new application method for asymmetrical silicon-metal dimer catalysts.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Review
Chemistry, Inorganic & Nuclear
Guanling Yang, Pengfei Zhou, Jinsheng Liang, Hao Li, Fei Wang
Summary: Nitrate (NO3-) and nitrite (NO2-) ions are common health-threatening contaminants in water. Catalytic thermal reduction using molecular hydrogen as the reducing agent is a promising strategy to reduce nitrate and nitrite. This review summarizes the current stages of thermal nitrate and nitrite reduction, discusses the opportunities and challenges in drinking water and wastewater treatment, and highlights the importance of exploring the mechanistic insights and design guidelines for thermal reduction.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Multidisciplinary
Pengfei Wang, Kun Zhang, Hao Li, Jing Hu, Menglian Zheng
Summary: Efficient mass transfer in electrodes is crucial for battery charge and discharge processes. This study introduces a novel 3D electrode design using layered double hydroxides (LDHs) nanosheets array for flow batteries, which significantly enhances mass transport and ion adsorption. The designed LDH electrode demonstrates high voltage efficiency and energy efficiency even at ultra-high current densities. Molecular dynamics simulations confirm the improved ion transport facilitated by LDH materials. This study offers a new approach to enhance mass transfer in electrodes for alkaline flow batteries and other energy storage devices.
