Article
Chemistry, Multidisciplinary
Dong Cao, Zhirong Zhang, Yahui Cui, Runhao Zhang, Lipeng Zhang, Jie Zeng, Daojian Cheng
Summary: In this study, highly active catalysts consisting of high-density Pt and Ir single atoms anchored on Co(OH)(2) were constructed for green hydrogen production. The catalysts exhibited excellent catalytic activity and efficiency in alkaline water electrolysis, demonstrating great potential for practical applications.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Weiqiong Q. Zheng, Ran Zhu, Huijuan J. Wu, Tian Ma, Hongju J. Zhou, Mi Zhou, Chao He, Xikui K. Liu, Shuang Li, Chong Cheng
Summary: This review summarizes the recent progress in tailoring bond microenvironments on different supports and discusses the reaction pathways and performance advantages of different single-atom sites (SASs) structures for water electrolysis. The essence and mechanisms of how SAS structures influence electrocatalysis and the critical requirements for future developments are also discussed. Challenges and perspectives are provided to stimulate the practical and widespread utilization of SAS catalysts in water-splitting electrolyzers.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Physical
Peng Zhu, Xiang Xiong, Dingsheng Wang
Summary: Hydrogen production from water splitting using renewable electric energy is a key topic for achieving a carbon neutral future. Single atom catalysts (SACs) have emerged as a new frontier in catalysis, particularly in the hydrogen evolution reaction (HER), due to their high activity and excellent chemical selectivity. However, the influence of the neighboring coordinated atoms from the supports is often neglected in the classification of SACs. This review proposes a new classification method based on the type of supports and highlights the importance of the metal-support interaction and coordination environment. Structural designing strategies are also proposed to address the current challenges in SACs for HER.
Article
Chemistry, Physical
Giovanni Di Liberto, Luis A. Cipriano, Gianfranco Pacchioni
Summary: This article investigates the relationship between metal atoms and their surrounding environment in single atom catalysts (SACs). The numerical experiments reveal that changing the active site or the surrounding environment can lead to significant variations in catalytic activity. The implications of this conclusion for modeling studies of SACs are discussed.
Review
Chemistry, Multidisciplinary
Wenwen Gao, Shihuan Liu, Guangxun Sun, Chao Zhang, Yuan Pan
Summary: Selective hydrogenation is a crucial reaction in the fine chemical industry, and the activation of H-2 is a key step. Catalysts, particularly single-atom catalysts (SACs), have shown great potential in activating H-2 for selective hydrogenation due to their high atom utilization and uniform active sites. Further research is needed to design SACs with superior H-2-activating capabilities.
Article
Chemistry, Physical
Jingsong Xu, Rui Li, Xiayan Yan, Qingkai Zhao, Rongguang Zeng, Jingwen Ba, Qifa Pan, Xin Xiang, Daqiao Meng
Summary: In this study, single atom catalysts (SACs) were proposed as promising catalysts for efficient hydrogen isotope separation by electrolysis of water. Pt SACs and Pt nanoparticles (NPs) were fabricated and their high activity and selectivity were attributed to the constructed Pt-N2C2 structure according to density functional theory calculations.
Review
Chemistry, Physical
Jingqi Guan, Xue Bai, Tianmi Tang
Summary: The review explores feasible design strategies for fabricating carbon-free single-site catalysts for hydrogen and oxygen evolution reactions, detailing the constitutive relationships between structure, composition, and catalytic performance. Insights are provided for constructing high-performance electrocatalysts for HER and OER, with future research directions and challenges in single-site catalysts for electrochemical water splitting suggested.
Article
Chemistry, Physical
Nuha Wazzan, Prafulla K. Jha
Summary: This study explores the potential of C18 nanoclusters and its analogous structures as SACs in the hydrogen evolution reaction and oxygen evolution reaction. It is found that there is a strong binding between transition metals and nanoclusters. The introduction of Ni, Pd, and Pt onto the nanoclusters improves the conductivity of the support, and exhibits potential as HER catalysts.
SURFACES AND INTERFACES
(2023)
Review
Chemistry, Physical
Mengyang Zhang, Keyu Xu, Ning Sun, Yanling Zhuang, Longlu Wang, Dafeng Yan, Bo Weng
Summary: This article reviews the application of bimetallic single-atom catalysts in electrocatalytic and photocatalytic hydrogen evolution reactions. It highlights the unique configuration and synergistic effects of these catalysts. The review covers recent advances in bimetallic single-atom catalysts under acidic/alkaline conditions, as well as their application in photocatalysis on semiconducting carbon nitrides. An outlook is provided on the opportunities and challenges in controlling catalyst synthesis and understanding bimetallic interactions.
Review
Chemistry, Applied
Qi-Ni Zhan, Ting -Yu Shuai, Hui -Min Xu, Chen-Jin Huang, Zhi-Jie Zhang, Gao-Ren Li
Summary: This review introduces various methods for preparing single-atom catalysts and discusses their electrocatalytic applications. The future challenges and prospects of monatomic catalysts are also discussed.
CHINESE JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Multidisciplinary
Ya-Kun Lv, Kun Wang, Wen-Yan Sun, Peng Peng, Shuang-Quan Zang
Summary: A sustainable and universal one-step electrochemical synthesis strategy is used to prepare catalysts with various single atomic sites such as Pt, Au, Ir, Pd, Ru, Mo, Rh, and W, among which the as-synthetic Pt-based catalysts exhibit outstanding activity and stability in the electrocatalytic hydrogen evolution reaction, extending the implications of electrochemical synthesis and the design of advanced electro-synthesized catalysts.
Review
Chemistry, Physical
Xingyuan Gao, Qiuping Dai, Xihong Lu, Sibudjing Kawi
Summary: This paper reviews the reaction mechanisms of electro-catalytic hydrogen evolution reaction (HER) and the preparation methods for single atom catalysts (SACs) supported on carbons. It discusses the applications of non-noble metal-based SACs/C catalysts in HER and elaborates on the structure-performance relationships. The challenges and perspectives of electrolytic HER are also proposed.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Nanoscience & Nanotechnology
Yang Liu, Jianghua Wu, Yuchen Zhang, Xu Jin, Jianming Li, Xiaoke Xi, Yu Deng, Shuhong Jiao, Zhanwu Lei, Xiyu Li, Ruiguo Cao
Summary: Hydrogen evolution reaction (HER) is crucial for electrochemical water splitting to produce hydrogen sustainably. However, the kinetics of HER is slow in neutral media, necessitating the use of noble metal catalysts. In this study, a catalyst comprising a single ruthenium atom (Ru1) and nanoparticles (Run) on a nitrogen-doped carbon substrate (Ru1-Run/CN) was developed, showing excellent activity and durability for neutral HER. The Ru1-Run/CN catalyst exhibited a low overpotential of 32 mV at 10 mA cm-2 and maintained stability for 700 hours at 20 mA cm-2. Computational calculations revealed that the presence of Ru nanoparticles in the catalyst improved the catalytic activity of HER by influencing the interactions between Ru single atom sites and reactants. This work highlights the ensemble effect of electrocatalysts for HER and provides insights for the rational design of efficient catalysts for other multistep electrochemical reactions.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Manjiao Chen, Xinqiang Yi, Xinjun Hu, Xinjun Zhou, Jianping Tian, Xiulan Li
Summary: Transition metal-doped graphene single-atom catalysts have great potential for catalyzing hydrogen evolution applications. The correlation between the catalytic activity of the central atom and the coordination environment is crucial. This study systematically explored the correlation between coordination environment and stability, catalytic activity of Fe-doped graphene catalysts. The results provide important insights for regulating the activity of single-atom catalysts.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Engineering, Environmental
Minghui Cui, Feilong Wang, Wenqi Zhao, Dai Zhang, Rongqing Liang, Qiongrong Ou, Shuyu Zhang
Summary: Green hydrogen is produced by electrolyzing water using renewable energy, thereby generating hydrogen with zero carbon emissions. Platinum-based catalysts are highly efficient, but limited by their high price and low availability. Researchers have synthesized a catalyst combining platinum single atoms and nanoparticles using nonthermal plasma technique, which exhibits excellent performance at high current density and a significantly lower loading compared to commercial catalysts. This technique offers a low-cost and efficient method to synthesize high-current hydrogen evolution reaction catalysts, promoting their industrial development.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Rui Liu, Zhichao Gong, Minmin Yan, Gonglan Ye, Huilong Fei
Summary: In this study, we demonstrate the fabrication of a monolithic aligned porous carbon film electrode co-modified with Pt single atoms and Pt nanoclusters through a simple electrochemical deposition process. This electrode exhibits outstanding performance for the hydrogen evolution reaction (HER) in sulfuric acid, with exceptional intrinsic and mass activity, as well as the ability to deliver high industrially relevant current density at low overpotential.
Article
Chemistry, Physical
Brandon C. Vance, Pavel A. Kots, Cong Wang, Jack E. Granite, Dionisios G. Vlachos
Summary: In this study, we report the application of a new and inexpensive catalyst Ni/SiO2, which can convert polyethylene into valuable n-alkane products under mild conditions. We reveal a new mechanism of long-alkane hydrogenolysis and demonstrate that the catalyst can handle multiple plastics, broadening the scope of catalysts for polyolefin hydrogenolysis and unleashing the potential for managing plastic waste.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Multidisciplinary
Jianbin Liu, Jiangwen Liao, Kang Huang, Juncai Dong, Guanchao He, Zhichao Gong, Huilong Fei
Summary: Metal- and nitrogen-doped nanocarbons (M-N-Cs) are promising alternatives to precious metals for catalyzing electrochemical energy conversion processes. However, M-N-Cs synthesized by high-temperature pyrolysis frequently suffer from compositional heterogeneity with the simultaneous presence of atomically dispersed M-N-x sites and crystalline metal nanoparticles (NPs), which hinders the identification of active sites and rational optimization in performance. A universal and efficient strategy is reported to obtain both precious- and nonprecious-metal-based M-N-Cs with exclusive atomic dispersion by using ammonium iodide as the etchant to remove excessive metal aggregates at high temperature.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Fanle Bu, Chaoqiu Chen, Yu Yu, Wentao Hao, Shichao Zhao, Yongfeng Hu, Yong Qin
Summary: A profound understanding of the nature of nuclearity effects is crucial for designing high-performance sub-nanocatalysts with low nuclearity, yet it remains a longstanding challenge. By employing atomic layer deposition, we precisely synthesized Fe sub-nanocatalysts with adjustable nuclearity (Fe-1-Fe-4) immobilized on N,O-co-doped carbon nanorods (NOC). The nuclearity-dependent electronic properties and spin configuration of the Fe sub-nanocatalysts dominate the activation modes of H2O2 and the adsorption strength of active O species on Fe sites for C-H oxidation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Shenglu Lu, Yaxuan Jing, Shengchao Jia, Mohsen Shakouri, Yongfeng Hu, Xiaohui Liu, Yong Guo, Yanqin Wang
Summary: The influence of Ru chemical state on the positions of C-C bond cleavage was investigated. Positively charged Ru species were found to favor the hydrogenolysis of the internal C-secondary-C-secondary bond, inhibiting methane production. A Ru/CeO2-I catalyst with plenty of Ru delta+ species was designed and proved efficient for the hydrogenolysis of real waste polyethylene plastics. This work will guide catalyst design to enhance the selective production of liquid alkanes.
Article
Multidisciplinary Sciences
Minmin Yan, Zengxi Wei, Zhichao Gong, Bernt Johannessen, Gonglan Ye, Guanchao He, Jingjing Liu, Shuangliang Zhao, Chunyu Cui, Huilong Fei
Summary: The researchers synthesized a material with high-density (10.32 wt%) single atoms of antimony (Sb) on nitrogen- and sulfur-codoped carbon nanofibers using a nanoarchitectured Sb2S3 template. This material exhibited high selectivity (97.2%) and mass activity (114.9 A g(-1)) for the 2e(-) ORR in alkaline electrolyte. Experimental and theoretical calculations showed that the coordination configuration and S dopants contributed to the enhanced activity and selectivity of the material.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Jingjing Liu, Zengxi Wei, Zhichao Gong, Minmin Yan, Yongfeng Hu, Shuangliang Zhao, Gonglan Ye, Huilong Fei
Summary: Doping phosphorus into the carbon substrate of a Co-N-C catalyst enhances the catalytic performance for the oxygen reduction reaction (ORR) and improves the selectivity for H2O2 electrosynthesis. The P-doped Co-N-C catalyst shows outstanding ORR activity with an early onset potential, high selectivity, and large turnover frequency in alkaline electrolyte, surpassing previously reported counterparts. In addition, as a gas diffusion layer in a flow cell, the catalyst achieves an unprecedented H2O2 production rate with long-term durability.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Green & Sustainable Science & Technology
Fahimeh Esmi, Ajay K. Dalai, Yongfeng Hu
Summary: Functionalized mesoporous aluminosilicates were synthesized using two different techniques of post and direct functionalization. Heteropoly acid was immobilized on the carriers and their performance for transesterification reaction was studied. The catalysts were analyzed for their properties and the direct functionalized catalyst with amino group showed higher catalytic activity and reusability compared to the one with thiol group.
JOURNAL OF CLEANER PRODUCTION
(2023)
Article
Green & Sustainable Science & Technology
Yongqing Bai, Zonglun Cao, Yongfeng Hu, Jing Zhao, Huaihao Zhang
Summary: In this study, a thermoconductive lignin-based hydrogel CaLS-CTS/h-BN was designed and synthesized for thermal energy conservation and soil self-remediation in thermal recovery of heavy oil. The gel improved the thermal efficiency and cumulative oil-steam ratio of steam flooding, reduced input energy, and enhanced heating profile and heat transfer. It also facilitated the biodegradation of the gel, alleviated formation damage, and increased the degradation of petroleum pollutants in soil. Additionally, it chelated and immobilized heavy metal contaminants in oilfield soil. This study provided a green adjuvant agent for cleaner production of heavy oil.
JOURNAL OF CLEANER PRODUCTION
(2023)
Article
Chemistry, Physical
Priya Karna, Zou Finfrock, Junjie Li, Yongfeng Hu, Dong-Sheng Yang
Summary: Copper has been widely used as a cost-effective and environmentally friendly metal catalyst in cross-coupling reactions. This article presents a water-soluble active molecular catalyst for Suzuki-Miyaura cross-coupling reactions using copper iodide as the precatalyst. The catalyst, identified as Cu(OH) in its singlet electronic state, is stable for at least 4 weeks in aqueous solutions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Zhichao Gong, Jingjing Liu, Minmin Yan, Haisheng Gong, Gonglan Ye, Huilong Fei
Summary: A high-performance seawater electrolysis catalyst, NiFe@DG, has been developed using a microwave shocking strategy. This catalyst exhibits low overpotentials and stable current density output in alkalized seawater, and maintains its activity with minimal decay after continuous operation for 2000 hours.
Article
Chemistry, Multidisciplinary
Xinyu Zhang, Yuyang Shi, Zude Shi, Hang Xia, Mingyu Ma, Yiliu Wang, Kang Huang, Ye Wu, Yongji Gong, Huilong Fei, Yongmin He, Gonglan Ye
Summary: High-quality SnS nanoribbons with an atomic thickness and anisotropic characteristics can be synthesized through high-pressure and thermal treatment methods. These nanoribbons have a length of several tens of micrometers and a thickness as low as 5.8 nm. They exhibit crystal orientation along the zigzag direction and in-plane structural anisotropy. A field-effect transistor fabricated with these nanoribbons shows high on/off current ratio and field-effect mobility.
Article
Chemistry, Physical
Siyu Wang, Xinran Ning, Xiaohui Liu, Mohsen Shakouri, Yongfeng Hu, Haiyang Yuan, Pengfei Liu, Xunyu Lu, Yong Guo, Yanqin Wang
Summary: This study reports a novel HER catalyst with oxygen-rich nitrogenated carbon synthesized from renewable lignin and low-cost melamine as the catalyst support. The catalyst exhibits low overpotential and excellent stability, demonstrating the crucial role of oxygen in nitrogenated carbon for HER and providing a strategy for developing high-efficient HER catalysts.
Article
Chemistry, Multidisciplinary
Jing Zhang, Yufeng Zhao, Wanting Zhao, Jing Wang, Yongfeng Hu, Chengyu Huang, Xingli Zou, Yang Liu, Dengsong Zhang, Xionggang Lu, Hongjin Fan, Yanglong Hou
Summary: A spin transition in a Mg-Fe dual-site catalyst is achieved by taking advantage of the local crystal field distortion induced by the large ionic radii difference between Fe/Mg. The as-synthesized catalyst demonstrates a low overpotential of 224 mV at 10 mA cm-2 for oxygen evolution reaction and an electrolysis voltage of only 1.542 V at 10 mA cm-2 for the overall water splitting.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
