Review
Chemistry, Multidisciplinary
Hui Xu, Junru Li, Xianxu Chu
Summary: This paper summarizes the recent progress in the field of hydrogen spillover in electrocatalytic hydrogen evolution reaction (HER), focusing on advanced strategies to intensify hydrogen spillover. The challenging issues and future development perspectives for hydrogen spillover-based electrocatalysts are also systematically discussed.
Article
Chemistry, Multidisciplinary
Shizheng Zhou, Haeseong Jang, Qing Qin, Liqiang Hou, Min Gyu Kim, Shangguo Liu, Xien Liu, Jaephil Cho
Summary: In this study, a Ru cluster anchored on a trace P-doped defective TiO2 substrate (Ru/P-TiO2) was synthesized as an electrocatalyst for the hydrogen evolution reaction (HER) in alkaline media. The Ru/P-TiO2 exhibited superior activity compared to commercial Pt/C and Ru/TiO2 materials. Experimental and theoretical studies revealed that the rutile-TiO2 crystal phase substrate with rich surface oxygen vacancies facilitated water adsorption and dissociation, while P substitution enhanced hydrogen generation by promoting hydrogen spillover, synergistically enhancing the HER activity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Yang Zhang, Xin Xiao, Xikui Wang, Xingxing Jiang, Xiaowu Gao, Peize Li, Yan Shen
Summary: Efficient and stable electrocatalysts for alkaline water splitting have attracted attention for cost-effective hydrogen production. Ni2P nanosheets arrays decorated with ruthenium nanoparticles on a carbon cloth substrate show good electrical conductivity and superior hydrophilicity. The resulting RuNi2P/CC-5 exhibits ultra-low overpotential and good long-term stability, providing a reasonable design route for efficient electrocatalyst in alkaline solution.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Hongyan Ji, Xiao Wang, Xiaoxu Wei, Yuxuan Peng, Shuaishuai Zhang, Shuyan Song, Hongjie Zhang
Summary: Hydrogenolysis is an effective method for converting polyolefins into high-value chemicals. In this study, the activity of CeO2-supported Ru single atoms, nanoclusters, and nanoparticles in LDPE hydrogenolysis showed a volcanic trend. Metal-support interactions and hydrogen spillover effect were identified as the two key factors in the reaction. Only when the balance between these two effects is achieved, as in CeO2-supported Ru nanoclusters, can the hydrogenolysis activity be promoted.
Review
Engineering, Environmental
Mengzhu Li, Weinan Yin, Junan Pan, Yanwei Zhu, Ning Sun, Xinyu Zhang, Yingtong Wan, Zhongzhong Luo, Lanhua Yi, Longlu Wang
Summary: Hydrogen spillover, a phenomenon of active species migration, has received considerable attention in recent years. It not only participates in catalytic reactions as reactants, but also induces support to form defects or phase transitions, thereby adjusting the energy band and improving catalytic performance. As a result, hydrogen spillover has broad potential applications in heterogeneous catalysis and hydrogen production. However, there is still a lack of clear summary on the reaction mechanism and important applications of hydrogen spillover. This review focuses on the recent progress of hydrogen spillover, including different types, structural models, and applications, aiming to provide new ideas for the design and application of hydrogen spillover.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Environmental
Junyu Zhang, Jianshe Lian, Qing Jiang, Guoyong Wang
Summary: The development of cheap and efficient OER/ORR/HER electrocatalysts is crucial for promoting green energy conversion and storage technologies. The Ru-doped NiO/Co3O4 heterostructure exhibits superior catalytic performance and stability.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Jinkyu Park, Honghui Kim, Seongbeen Kim, Seung Yeop Yi, Hakyung Min, Daeeun Choi, Seonggyu Lee, Jihan Kim, Jinwoo Lee
Summary: This study reports the design of Ru single-atom catalyst supported on tungsten carbide, which exhibits remarkably enhanced performance in alkaline hydrogen oxidation reaction by promoting hydroxyl adsorption on the interface. This work provides new insights into the design of highly active SACs for alkaline HOR.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Jiahe Peng, Zhongyong Zhang, Hao Wang, Peng Zhang, Xiujian Zhao, Yu Jia, Yuanzheng Yue, Neng Li
Summary: The emergence of amorphous 2D materials has opened up new avenues for materials science and nanotechnology. However, there have been no reports on amorphous MXene materials. In this study, a unique amorphous Ti2C-MXene model was built using ab initio molecular dynamics approach. The structure analysis showed a composited structure of a-Ti2C-MXene, which exhibited high activity for boosting hydrogen evolution reaction performance. This work provides insights for future research on novel MXene materials.
Article
Engineering, Environmental
Qi Cao, Shuang Hao, Yunwen Wu, Ke Pei, Wenbin You, Renchao Che
Summary: The binder-free Ni2P-Co2P/CC electrocatalyst exhibits outstanding HER activity in alkaline and acidic conditions, attributed to abundant interfacial contact, regulated electronic structure, hydrophilic surface, and interfacial charge redistribution contributing more high-valence Ni active sites. This work demonstrates the potential of facile strategy for the design and preparation of highly efficient phosphide electrocatalysts.
CHEMICAL ENGINEERING JOURNAL
(2021)
Review
Chemistry, Inorganic & Nuclear
Xianxu Chu, Junru Li, Hui Xu, Weiyu Qian
Summary: This article summarizes the recent progress and applications of Te-based nanocatalysts in electrocatalytic reactions. The positive influence of Te on electrocatalysts includes serving as a template for nanostructure construction, modifying electronic structure, and increasing surface defect density, leading to optimized electrocatalytic performance.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Arumugam Sivanantham, Hansung Lee, Sung Won Hwang, Han Uk Lee, Sung Beom Cho, Byungmin Ahn, In Sun Cho
Summary: This study investigates the active role of vanadium in improving the electrocatalytic activity for the hydrogen evolution reaction in VxCuCoNiFeMn (x = 0, 0.5, and 1.0) high entropy alloys. The incorporation of vanadium enhances the electrical conductivity and electrochemical surface area of the alloy, leading to improved kinetics for the reaction. The findings can contribute to the development of highly active high entropy alloys for large-scale electrochemical water splitting.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Review
Chemistry, Physical
Chongao Tian, Rui Liu, Yu Zhang, Wenxiu Yang, Bo Wang
Summary: Electrolytic water splitting is a feasible and promising technique for hydrogen energy production, but the slow kinetic rate of hydrogen/oxygen evolution reactions leads to high overpotential and low energy efficiency. Pt/Ir-based nanocatalysts have become the state-of-the-art catalysts, but their high cost and low earth abundance limit their applications. Ru-based nanomaterials, particularly Ru-doped functional porous materials, have attracted attention for their low price, Pt-like hydrogen bond strength, and high EWS activity. This review summarizes the design and preparation strategies of Ru-doped functional porous materials for EWS, as well as the structure-activity relationships induced by the tuned geometric/electronic structures. The challenges and perspectives of Ru-doped functional porous materials catalysts are also proposed.
Article
Chemistry, Multidisciplinary
Yuanmeng Zhao, Xuewei Wang, Zhen Li, Pingping Zhao, Congliang Tao, Gongzhen Cheng, Wei Luo
Summary: This study presents a new strategy to enhance the electrocatalytic performance of ruthenium nanoparticles for hydrogen oxidation and hydrogen evolution reactions in alkaline media through nitrogen modification. The nitrogen-modified ruthenium nanoparticles exhibit remarkable catalytic performance, outperforming both the untreated ruthenium nanoparticles and commercial platinum catalysts. The enhanced performance is attributed to the electronic regulation of ruthenium after nitrogen incorporation, optimizing the hydrogen adsorption Gibbs free energy.
CHINESE CHEMICAL LETTERS
(2022)
Article
Engineering, Environmental
Xiaofeng Zhang, Xiaocui Li, Zhangweihao Pan, Yongjian Lai, Yang Lu, Yi Wang, Shuqin Song
Summary: By introducing crystal defects, the adsorption capability of electrocatalysts is optimized to enhance the hydrogen evolution reaction (HER) activity significantly. The defect-rich Ni nanoparticles wrapped by few-layer graphene are uniformly fixed on the conductive carbon network, effectively preventing aggregation and peeling off, providing good stability for HER.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Nanoscience & Nanotechnology
Caihua Zhang, Fengyan Han
Summary: A hollow Ru nanostructure (h-RuNP) was developed as a highly efficient and stable Pt-free electrocatalyst for the hydrogen evolution reaction. It demonstrated superior catalytic activity and long-term stability compared to pure Ru and Ru-based nanocatalysts, approaching that of commercial 20% Pt/C catalyst. The enhanced performance of h-RuNP was attributed to the strong surface oxidation resistance and antiaggregation effect of unsupported ultrasmall Ru nanoparticles.
ACS APPLIED NANO MATERIALS
(2021)
Article
Engineering, Environmental
Yubo Liu, Xiaofei Cao, Jiakun Shi, Binbin Shen, Jianying Huang, Jun Hu, Zhong Chen, Yuekun Lai
Summary: In this study, a superhydrophobic coating with excellent mechanical durability and chemical stability was successfully prepared by in-situ growing SiO2 particles on the surface of carbon nanotubes and modifying them with thermoplastic polyurethane matrix. The coating has multi-level micro/nanostructures and strong bonding, which prevent the adhesion of contaminants on the coating surface and in liquids, and also exhibit self-cleaning and anti-fouling properties.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Tingting Cai, Chao Liu, Jie Liang, Yan Ma, Jun Hu, Jianchun Jiang, Kui Wang
Summary: This study proposes a new perspective on the design of a biphasic system from a polar aprotic solvent (PAS) and saline water, based on the studies on intermolecular weak interactions. Molecular dynamics simulation reveals the formation mechanism of the biphasic system, and the stronger interaction of Na+ and Cl- with water is proven to be responsible for the dissociation of water from water-miscible gamma-valerolactone (GVL). The excellent extraction and stabilization of furfural (FAL) in the biphasic system can be attributed to the better interaction of PAS with FAL.
Article
Chemistry, Physical
Sai Zhang, Zhaoming Xia, Wenbin Li, You Wang, Yong Zou, Mingkai Zhang, Zhongmiao Gong, Yi Cui, Yongquan Qu
Summary: We found that single-atom Pt on Co304 undergoes in-situ reconstruction to form isolated Pt-Co bimetallic sites, reducing the coordination number of Pt-O in the presence of hydrogen. This modified chemical state of Pt greatly enhances H2 activation, leading to a significantly higher turnover frequency for the hydrogenation of cinnamaldehyde compared to Pt nanoparticles on Co304. The high selectivity towards cinnamyl alcohol is attributed to a tilted adsorption configuration of the reactant on the catalyst surface via the aldehyde group. Our findings on the in-situ reconstruction of single-atom catalysts under reducing conditions have important implications for the design of highly efficient hydrogenation catalysts.
Article
Chemistry, Multidisciplinary
Mingkai Zhang, Sai Zhang, Yuanyuan Ma
Summary: This study demonstrates a facile and efficient strategy for the preparation of cobalt catalysts through in situ reconstruction of cobalt borate during the reductive amination. The cobalt borate is transformed into cobalt hydroxide through interaction with ammonia and subsequently reduced to cobalt nanoparticles by hydrogen under reaction conditions. The in situ generated cobalt catalysts exhibit excellent catalytic activity and selectivity, surpassing commonly used cobalt/carbon, platinum, or Raney nickel catalysts. It is anticipated that this new strategy of in situ reconstruction of cobalt borate could provide a new approach for the design and optimization of catalysts to produce primary amines.
FRONTIERS IN CHEMISTRY
(2023)
Article
Nanoscience & Nanotechnology
Yu Sun, Bing Du, You Wang, Mingkai Zhang, Sai Zhang
Summary: Hydrogen spillover allows the design of dual-active site catalysts for selective hydrogenation. This study demonstrates selective hydrogenation dependent on hydrogen spillover on WO3-supported Pd catalysts. The WO3 supports with a hexagonal phase and suitable oxygen defect concentration enhance the capacity of hydrogen spillover, significantly improving the catalytic activity. This work contributes to the development of cost-effective nanocatalysts with low Pd loading for highly active and selective hydrogenation.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
You Wang, Bing Liu, Qing Guo, Yu Sun, Sai Zhang, Yongquan Qu
Summary: K+-doped Pt nanoparticles on γ-Al2O3 (PtKx/Al2O3) stabilized the *OH intermediates on Pt surface, achieving efficient H2 generation with ultra-low levels of CO through APRM at 120 degrees C. These findings are anticipated to promote methanol as a practical H2 carrier for the delivery of hydrogen with high purity.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Sai Zhang, Zhimin Tian, Yuanyuan Ma, Yongquan Qu
Summary: The adsorption of molecules on CeO2-based catalysts greatly influences their catalytic performance. By regulating the oxygen defect of CeO2, two active sites, frustrated Lewis pair and dual-active site, can be constructed, which enhance the catalytic activity and selectivity. The unique spatial and electronic structures of the active sites promote the activation and transformation of small molecules, and the dual-active sites enable highly active and selective hydrogenations by breaking the competitive adsorption. The possibilities and challenges in the adsorption behaviors of various molecules on CeO2-based catalysts are also outlined.
Article
Chemistry, Multidisciplinary
Yanfeng Shi, Gong Zhang, Chao Xiang, Chengzhen Liu, Jun Hu, Junhu Wang, Rile Ge, Haixia Ma, Yusheng Niu, Yuanhong Xu
Summary: This study demonstrates the potential of achieving a sustainable heterogeneous Fenton system by enhancing the ligand-to-metal charge-transfer (LMCT) excited-state lifetime in an Fe-gallate complex. The improved excited-state lifetime leads to efficient Fe cycles and enhanced H2O2 activation kinetics and hydroxyl radical (center dot OH) productivity. Furthermore, the system shows promising catalytic activity and stability, with implications for designing efficient and sustainable Fenton-like processes.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Wenbin Li, Jie Gan, Yuxuan Liu, Yong Zou, Sai Zhang, Yongquan Qu
Summary: In this study, a dual-active site catalyst comprising Pt clusters and frustrated Lewis pairs on porous CeO2 nanorods was developed for the low-temperature reverse water-gas shift (RWGS) reaction. The Pt clusters effectively activated hydrogen, while the frustrated Lewis pair sites enhanced CO2 adsorption and weakened CO adsorption to facilitate CO release and suppress CH4 formation. The catalyst showed high CO yield close to thermodynamic equilibrium and a large turnover frequency, demonstrating its potential for optimizing the RWGS reaction.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Applied
Xiaofei Cao, Siqian Xing, Duo Ma, Yuan Tan, Yucheng Zhu, Jun Hu, Yao Wang, Xi Chen, Zhong Chen
Summary: Rational design of high-performance electrocatalysts for hydrogen evolution reaction (HER) is crucial for future renewable energy systems. This study developed a multi-level screening methodology to search for stable and active dopants for CoP catalysts. Theoretical and experimental results showed that the difference in work function (Delta phi) and the d-band center (d-BC) of the doped system play important roles in regulating the adsorption free energy (Delta G(H*)) of HER. The discovery of these regulatory parameters can drive the development of high-performance ion-doped electrocatalysts for electrocatalytic water splitting.
JOURNAL OF ENERGY CHEMISTRY
(2023)
Article
Nanoscience & Nanotechnology
Enxiang Ren, Xing Zhang, Guo-Ping Lu, Muhammad Sohail, Jun Hu, Zhong Chen, Daidi Fan, Yamei Lin
Summary: The poor activity and specificity of nanozymes due to low density of active sites, inhomogeneous atomic composition, and complex structure can be overcome by the fabrication of a single iron-anchored carbon material, Fe/CN-800-A, with FeN2 sites, which exhibits exclusive oxidase-like activity. The mechanisms of N-coordination-number-regulated enzymatic activity and specificity of the composite are explored to understand the working principle. The FeN2 sites in Fe/CN-800-A have higher oxidase-like activity and specificity compared to the FeN4 sites in Fe/CN-700, thanks to their lower energy barriers for O-2 absorption and decomposition of H2O2 into O-2. These findings provide a theoretical basis for the rational design of nanozymes with high oxidase-like activity and specificity, with potential commercial applications in chlorpyrifos detection and antibacterial applications.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Ke Xu, Yu Sun, You Wang, Bing Du, Xiaolong Li, Sai Zhang
Summary: We found that the catalytic activity of benzoic acid hydrogenation to cyclohexanecarboxylic acid is influenced by the initial surface fraction of Pd2+ in Pd nanoparticles. Additionally, we proposed a mechanism for the deactivation of Pd/C catalyst in benzoic acid hydrogenation, which involves a decrease in the fraction of Pd2+ in a strongly reducing atmosphere.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Wenbin Li, Junhao Ding, Xiao Chen, You Wang, Xu Song, Sai Zhang
Summary: This study presents a monolithic CuNi alloy catalyst with ordered microchannels and a unique lattice structure fabricated using 3D printing technology. The catalyst exhibits enhanced mass and heat transfer efficiencies and shows excellent catalytic performance and stability in the reverse water-gas shift reaction.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Yong Zou, Zhaoming Xia, You Wang, Yuxuan Liu, Sai Zhang, Yongquan Qu
Summary: This article describes the reconstruction of frustrated Lewis pair (FLP) site on the CeO2(110) surface to form (La, Ce)-O upon La-doping. The (La, Ce)-O FLP site with tailored local Lewis acid-base property and increased spatial distance between the Lewis acid and base facilitates the tandem transformation of styrene and CO2 through weakened adsorption of CO2 while maintaining activation.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Yong Zou, Yuxuan Liu, Sai Zhang, Yongquan Qu
Summary: This study successfully achieved efficient oxidation of toluene and condensation with malononitrile using cobalt-doped nanorods of ceria with dual active-sites. The presence of oxygen vacancies and cobalt species promoted the activation of both O2 and C(sp(3))-H, enabling the synthesis of benzylidenemalononitrile under mild conditions. Experimental and theoretical simulations revealed that the oxidation of C(sp(3))-H and condensation with malononitrile were facilitated by the spillover of active oxygen species and the presence of cobalt sites.
