Table of Content

10 January 2023, Volume 44 Issue 1

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Preface

中空结构材料专辑

王丹, 殷亚东, 余承忠, Andreu Cabot

2023, 44(1):  1-2. 

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Content

Cover and Content of Chemical Journal of Chinese Universities Vol.44 No.1(2023)

2023, 44(1):  1-6. 

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Account

Etching-based Hollowing of Nanostructures

YE Zuyang, YIN Yadong

2023, 44(1):  20220656.  doi:10.7503/cjcu20220656

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The controllable synthesis of hollow nanomaterials has broad application prospects in many fields， such as catalysis， energy conversion and storage， and biomedicine. This account aims to reveal the key effects of etching on the hollowing process of nanostructures. We discuss the precise manipulation of the hollowing process by enhancing the relative stability of the nanoparticle surface in the etchant， mainly focusing on three types of etching strategies， including the hard templating method， redox-assisted etching method， and surface-passivated etching method. Finally， we provide an outlook on the future development of etching-based strategies for the controllable synthesis of hollow nanostructures.



Review

Gate Keeper in the Smart Hollow Drug Carrier

WANG Hui, ZHAO Decai, YANG Nailiang, WANG Dan

2023, 44(1):  20220237.  doi:10.7503/cjcu20220237

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Recently， the unique and novel structure of hollow materials has become a hot spot in the research of synthetic chemistry and material chemistry， especially its high surface-volume-ratio， low density and large cavities， and it is also an excellent choice of drug delivery carrier. Through the precise selection and modification of hollow materials， the hollow materials can be endowed with unique stimulus response behavior， thus realizing the intelligent design of hollow materials and the controlled release of drugs. There are two strategies for constructing smart hollow carriers： （1） utilizing hollow materials as carriers that can respond to physical or chemical stimuli； （2） modifying functional molecules on the surface of hollow carriers to achieve specific “on-off” switch under stimulation. Its core lies in the precise regulation of molecular composition and configuration. From this perspective， we detail the construction connotation of gatekeepers for controlled drug release. This review begins with an introduction to the development history of hollow carriers， followed by a brief discussion on the rules of molecules released from hollow structures. The use of hollow structures for the construction of intelligent responsive drug carriers is then showcased， including roles of the hollow structure， different gating strategies， controlled release mechanisms， and their potential progress in application. This paper concludes with some perspectives on future directions for hollow structured carriers.



Recent Advances in Metal-organic Framework Derived Hollow Superstructures： Synthesis and Applications

ZOU Yingying, ZHANG Chaoqi, YUAN Ling, LIU Chao, YU Chengzhong

2023, 44(1):  20220613.  doi:10.7503/cjcu20220613

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Rational design of metal-organic framework（MOF） derived functional materials with elaborate structures is of great significance for diverse applications. Assembly of simple MOF derivatives as building blocks into hollow superstructures（HSSs） represents a promising strategy for creating higher-order structures with improved performance. Even many excellent reviews on MOF derivatives have been reported， a dedicated review from the angle of synthesis and applications of HSSs is still lacking. Here we provide a timely and systematic review on the recent advances of MOF derived HSSs. Firstly， five types of MOF derived HSSs are classified according to their architectural features. Then， the synthesis strategies for creating HSSs from MOF derivatives are summarized， with an emphasis on how to design MOF precursors and select conversion conditions. Afterwards， the promising applications of MOF derived HSSs in energy and catalysis related fields are highlighted. Finally， our perspectives on challenges and future opportunities in MOF-derived HSSs are presented， aiming to provide guidance for the design of advanced MOF derivatives with intricate structures and enhanced properties.



Intricate Hollow Structured Materials： Synthesis and Energy Applications

WU Yucai, DU Huan, ZHU Jiexin, XU Nuo, ZHOU Liang, MAI Liqiang

2023, 44(1):  20220689.  doi:10.7503/cjcu20220689

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The increasing energy demand makes it necessary to develop novel multifunctional materials to meet the requirements of energy storage and conversion. Among various functional materials， intricate hollow structured materials have received extensive attention due to their unique structure and physicochemical properties. In this review， the synthesis strategies and energy applications of intricate hollow structured materials are summarized. The synthesis strategies are mainly divided into five categories： hard templating， soft templating， self-templating， sequential templating and selective etching methods. The applications of intricate hollow structures include lithium-/sodium-/potassium-ion batteries， lithium-sulfur batteries， supercapacitors， electrocatalysis， photocatalysis and dye-sensitized solar cells. Finally， the existing problems and future research directions for intricate hollow structures are discussed.



Progresses in Template Synthesis and Applications of Hollow Materials

YANG Jiye, SUN Dayin, WANG Yan, GU Anqi, YE Yilan, DING Shujiang, YANG Zhenzhong

2023, 44(1):  20220665.  doi:10.7503/cjcu20220665

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Hollow materials are emerging as functional materials with unique characteristics in tunable cavity， high specific active surface area and enhanced mass transfer. Janus hollow materials are readily derived upon spatial compartmentalization of multiple components thus functions. Template synthesis is highly efficient to synthesize the hollow materials with tunable microstructure and composition. In the first part of this review， recent advances in the template synthesis of the representative hollow materials are concisely summarized. In the second part， typical applications of the hollow materials in catalysis， energy storage， oil/water separation and drug delivery are introduced. This review will end with a perspective to call for more efforts in the development of new methods toward high performance hollow materials with tailored properties.



Synthesis Strategies for Polymer Hollow Particles

SHEN Xinyi, ZHANG Sen, WANG Shutao, SONG Yongyang

2023, 44(1):  20220627.  doi:10.7503/cjcu20220627

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Polymer hollow particles have received much attention in the last two decades due to their unique structure and fascinating properties. They exhibit low density， large surface area， and high loading capacity properties， showing great promise in applications ranging from catalysts， drug delivery carriers， to energy storage. In this review， we summarize the synthesis strategies of polymer hollow particles， including templating synthesis， emulsion polymerization， self-assembly， microfluidics， and some other strategies. The synthesis principle， typical process， advantages， and disadvantages of these strategies have been elaborately illustrated and discussed. We also point out some challenges of existing strategies and some shortcomings of polymer hollow particles and provide an outlook on the future developments of the preparation and application of polymer hollow particles. We expect more strategies will be developed for the synthesis of polymer hollow particles with enhanced performance and multiple functions.



Synthesis Methods and Electrocatalytic Performance of Noble-metal Nanoframes Catalysts

KUANG Huayi, CHEN Chen

2023, 44(1):  20220586.  doi:10.7503/cjcu20220586

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Noble-metal nanoframes connected by ultrathin frames have attracted extensive attention in the field of heterogeneous catalysis due to their advantages of low loading capacity and high activity. The unique 3D open accessibility structure of the nanoframes can not only expose more active sites at the edges and vertices， improving the utilization rate of noble metal active sites， but also limit the reaction substrates to the nanoscale， increasing the chance of substrate molecules colliding. At present， researchers have proposed a variety of synthesis methods for noble-metal nanoframes， including crystal etching method， sacrificial template method， self-assembly method and so on. Their applications in catalysis and energy storage have also been explored. In this review， we summarized the synthesis strategies of noble metal nanoframes and their applications in the field of electrocatalysis in recent years， and put forward the prospect of its future development direction and challenges.



Current Advances of Hollow All-solid-state Z-Scheme Photocatalysts

LIU Shuanghong, XIA Siyu, LIU Shiqi, LI Min, SUN Jiajie, ZHONG Yong, ZHANG Feng, BAI Feng

2023, 44(1):  20220512.  doi:10.7503/cjcu20220512

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Hollow structural materials have great application value in photocatalytic applications due to their large specific surface area， low density and short charge transport distance. Z-Scheme photocatalysts have wide range of spectral response， high stability， high separation efficiency of photogenerated carriers， strong oxidation and reduction capabilities， have received widespread attention. However， due to the instability of Z-scheme multi- element structure and hollow structure， it is still a huge challenge to design efficient and stable hollow all-solid-state Z-scheme photocatalysts. In this review， we summarized and discussed the advances progress in the types， construction strategies and performance researches of hollow all-solid-state Z-scheme photocatalysts in recent years， and envisioned the problems and challenges on the future applications， which will provide references for the design of stable photocatalysts.



Recent Advances in Synthesis and Applications of Hollow Nano-carbons

WANG Sijia, HOU Lu, LI Chenglong, LI Wencui, LU Anhui

2023, 44(1):  20220637.  doi:10.7503/cjcu20220637

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Hollow nano-carbons have been attracting great attention due to their unique features such as low density， high surface-to-volume ratios， adjustable internal cavity and pore structures， etc. Here， we provide an overview of the preparation methods of hollow nano-carbons， including confined nanospace pyrolysis， hard-templated method， soft-templated method and so on. The recent advances of their applications in energy storage， catalysis， adsorption and biomedicine are summarized. Finally， some challenges on the controllable synthesis as well as their practical applications are outlined and the perspectives are proposed.



Design， Regulation and Applications in Lithium-sulfur Battery Cathodes of Yolk-shell Nanoreactors

WU Yujie, HUANG Wenzhi, PAN Junda, SHI Kaixiang, LIU Quanbing

2023, 44(1):  20220619.  doi:10.7503/cjcu20220619

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Lithium-sulfur batteries have attracted much attention due to their high theoretical energy density， which are considered as one of the most promising class of new secondary batteries. In view of the sulfur cathode， there are problems such as the insulation properties of sulfur and lithium sulfide， the diffusion of soluble polysulfides， the volume expansion of sulfur in the cycle process， and the slow dynamics of the redox process， which seriously restricts the activity and cycle stability of the lithium-sulfur battery. Yolk-shell nanoreactors， with easy to regulate “yolk”， “shell”， and “void”， can alleviate the electrode volume in the process of charge and discharge change， provide fast ion/electron transport channel， strengthen polysulfide adsorption and improve catalytic conversion reaction， etc.， thus significantly improve the electrode stability， activity and cycle performance， conducive to promoting the commercialization process in lithium sulfur battery. Thus， we summarize the design and regulation strategy of yolk-shell nanoreactors， including single-yolk-single-shell， single-yolk-multi-shell， multi-yolk-single-shell and multi-yolk-multi-shell. Furthermore， combined with the working characteristics and current application problems of lithium-sulfur battery， the application prospect and future development are also discussed.



Research Progress of Hollow Metal-organic Frameworks

LU Yu, WANG Tie

2023, 44(1):  20220662.  doi:10.7503/cjcu20220662

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The rapid development of hollow metal-organic frameworks（HOMOFs） has opened up new application fields for hollow structural materials. This review introduced the preparation methods of HOMOFs， focusing on the applications of HOMOFs and their composites， including catalysis， photocatalysis and electrocatalysis， adsorption， gas separation， sensing， supercapacitors， and biomedicine. At the same time， the preparation and application of specific HOMOFs and their composite materials were also elaborated. Finally， the opportunities and challenges faced by HOMOFs materials were prospected.



Progress of Hollow Carbon Materials as Anode for Sodium-ion Battery

ZHANG Lingling, DONG Huanhuan, HE Xiangxi, LI Li, LI Lin, WU Xingqiao, CHOU Shulei

2023, 44(1):  20220620.  doi:10.7503/cjcu20220620

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Achieving the large-scale application of energy storage devices such as sodium-ion batteries（SIBs）， is a great significance for the sustainable development of energy and the achievement of the goal of “peak carbon dioxide emissions and carbon neutrality”. The key factor of the large-scale application of SIBs is developing high-performance anode materials with improved energy density， rate performance and cycle stability. Hollow carbon materials（HCMs） has a wide application prospect as anode for SIBs due to its excellent rate performance and cycle stability caused by unique structure. Herein， this review summarizes the synthetic methods of HCMs and the relationship between their morphology， heteroatom modification strategy and sodium storage properties comprehensively， and looks into the future development of HCM.



Application of Electrospun Hollow Nanofibers in Catalysis

LI Huaike, YUE Guichu, XIE Haiyun, LIU Jing, GAO Songwei, HOU Lanlan, LI Shuai, MIAO Beibei, WANG Nyu, BAI Jie, CUI Zhimin, ZHAO Yong

2023, 44(1):  20220625.  doi:10.7503/cjcu20220625

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Larger specific surface area， richer interfacial composition， and more efficient mass transfer paths are the keys to constructe multi-component catalytic systems and improve catalyst efficiency. Hollow nanofibers with multiple cavity structures show great capability to adjust their specific surface area and interface composition， and become an ideal platform for preparing highly efficient heterogeneous catalysts. The development of electrospinning technology provides a simple and efficient method for the controllable preparation of hollow nanofibers， and effectively promotes the structural innovation and application expansion of hollow nanofibers. In this review， the unique advantages of hollow nanofiber materials with different composition and morphology prepared by electrospinning in the application of catalysis（including photocatalysis， electrocatalysis and thermocatalysis） are summarized from three aspects： construction strategies， structural characteristics and the corresponding relationship between structure and performance. Firstly， the different structural forms of hollow nanofibers prepared by innovative electrospinning methods combined with subsequent processes are demonstrated， and then the research progress of constructing high-efficiency catalysts based on hollow nanofibers are reviewed. Finally， the future development trends of the applications of hollow nanofibers in the field of catalysis are summarized and prospected to provide a useful reference for the design of high-efficient heterogeneous catalysts.



Progress on Preparation and Electrocatalytic Application of Hollow MOFs

YANG Qingfeng, LYU Liang, LAI Xiaoyong

2023, 44(1):  20220666.  doi:10.7503/cjcu20220666

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Water splitting， metal-air batteries and fuel cells are energy conversion technologies that are critical to solving future energy crises and environmental problems. The oxygen reduction reaction（ORR）， oxygen release reaction（OER） and hydrogen release reaction（HER）， as the core reactions， have the problem of slow kinetic speed， so it is of great significance to develop efficient non-noble metal electrocatalysts. Metal-organic frameworks（MOFs） have attracted more and more attention in different applications due to their highly tunable compositions and porous crystal structures. And hollow MOFs have the advantages of highly adjustable composition and structure of MOFs， as well as the advantages of hollow structure nanomaterials， such as faster transmission quality， more abundant porosity， rich active components， more exposed active sites， and better compatibility with harsh conditions， etc.， and show great potential applications in the field of electricity catalysis. In this paper， the preparation of hollow MOFs based structural materials and their research progress in electrocatalysis in recent years are reviewed， and the challenges and prospects in this field are summarized.



Progress in the Structure Design and Surface Manipulation of Lithium-rich Cathode Materials

ZHAO Xiaolang, YANG Mei, WANG Jiangyan, WANG Dan

2023, 44(1):  20220263.  doi:10.7503/cjcu20220263

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Lithium-rich cathode materials are regarded as promising cathode candidates for next-generation lithium-ion battery， due to their high theoretical energy density. However， the rapid capacity and voltage decay during cycling hinders their practical commercial application. In this review， the research progress of improving the lithium storage performance of lithium-rich cathode materials through structure design and surface manipulation was summarized in detail. Firstly， the working mechanism of charge and discharge of lithium-rich cathode materials as well as the reasons for their specific capacity and voltage decay were introduced. Subsequently， we discussed the recent progress in improving the performance of lithium-rich cathode materials through novel structural design and surface manipulation strategies. By constructing novel structure such as yolk-shell and hollow multishelled structure， and by controlling the particle size， exposing beneficial surface， surface spinelization， surface coating， surface doping， etc.， the surficial oxygen loss and crystal form transformation of the lithium-rich cathode materials could be effectively inhibited， and the geometric structure could be stabilized. As a result， the decay of voltage and specific capacity could be suppressed， and the cycle life and Coulomb efficiency of the battery could be improved. Finally， the remained challenges of improving the electrochemical performance of lithium-rich cathode materials are discussed and the future development directions are prospected.



Article

Iron Phthalocyanine Coated Nitrogen-doped Hollow Carbon Spheres for Efficient Catalysis of Oxygen Reduction Reaction

LI Ziruo, ZHANG Hongjuan, ZHU Guoxun, XIA Wei, TANG Jing

2023, 44(1):  20220677.  doi:10.7503/cjcu20220677

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It is imperative to develop low-cost and high-performance catalysts for oxygen reduction reaction（ORR）. Although iron phthalocyanine（FePc） has been proved as an efficient catalyst for ORR decades ago， it cannot replace commercial Pt/C due to its poor electronic conductivity and unsatisfied stability. Considering the chemical stability， high electronic conductivity， and intrinsic catalytic activity of nitrogen-doped carbons， herein， FePc coated nitrogen-doped hollow carbon（FePc-NHC） has been fabricated by carbonization of polystyrene@polydopamine spherical precursors， followed by the loading of FePc. A series of hollow spherical FePc-NHCS samples was prepared by adjusting the pyrolysis temperature and loading amount of FePc. Benefiting from the hierarchical porous structure， high specific surface area， proper nitrogen doping， and FePc loading， the optimized FePc-NHCS displayed an excellent catalytic activity for ORR in alkaline electrolyte， with a remarkable long-term stability and a high half-wave potential of 0.862 V（vs. RHE）， outperforming Pt/C（0.848 V）. This work proved that hybridization is an effective pathway to strength the positive properties of each component. Also， structural and compositional modification is efficient to optimize the ORR performance of a catalyst.



Synthesis and Lithium-ion Battery Performance of Hollow Multishelled CoFe₂O₄

BI Ruyi, ZHAO Jilu, WANG Jiangyan, YU Ranbo, WANG Dan

2023, 44(1):  20220453.  doi:10.7503/cjcu20220453

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Binary transition metal oxides have attracted significant attention as high-performance lithium ion battery electrode materials， due to their excellent electrochemical activities. However， the poor cycling stability of the material limits its practical application. In this study， we synthesized CoFe₂O₄ hollow multishelled structure（HoMS） material by sequential templating approach， and characterized its morphology and structure. In addition， the relationship between shell structure and battery performance is well studied. It is demonstrated that double-shelled core CoFe₂O₄ HoMS has the highest discharge capacity（1354.4 mA·h/g）， excellent rate performance and cycle stability. The outstanding electrochemical performance is mainly attributed to its unique structural advantages and optimal cavity volume occupancy， which enables it to maintain good structure stability and beneficial electrochemical properties during the repeated cycling.



Preparation and Microwave Absorbing Property of NiFe₂O₄/C Composites with Hollow Multishelled Structure

HUANG Tianye, YANG Mei, WANG Jiangyan, ZHANG Shaojun, DU Jiang, WANG Dan

2023, 44(1):  20220276.  doi:10.7503/cjcu20220276

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Hollow nickel ferrite（NiFe₂O₄） materials with single-shelled and double-shelled structures were synthesized by a facile sequential templating approach（STA） to obtain the lightweight and high-performance electromagne-tic wave absorbent. The morphology of NiFe₂O₄ was controlled by changing the slurry constituents and process parameters. Polydopamine（PDA） and carbon were designed and coated on the surface of NiFe₂O₄ through a simple in⁃situ polymerization and carbonization treatment， forming the composites with hollow multishelled structure（HoMS）. The electromagnetic parameters of NiFe₂O₄/C composites with different morphologies were measured by a network analyzer， and their reflection loss values were calculated by transmission line theory. And the effect of composites’ structures on the performance of electromagnetic absorbing were discussed in detail. The results show that the thin carbon coating significantly improves not only the electromagnetic properties but also the impedance matching， and thus the highly effective reflection loss. The double-shelled NiFe₂O₄/C HoMS composites displayed an excellent microwave absorbing performance. A minimum reflection loss（RL_min） of ‒32.35 dB was obtained at 8.44 GHz with absorber thickness of 3.5 mm， along with an effective absorption bandwidth of 3.68 GHz at a 2.0 mm thickness. These results can be attributed to the designable HoMS， which increases the probability of the multiple reflections/scattering and realizes more absorption of microwave besides the interfacial polarization between nanoparticles on the shells.



Salt-templated Synthesis and Morphological Control of Monodisperse Hollow Mesoporous Structures

ZHU Kerun, REN Wenxuan, ZHANG Wei, LI Wei

2023, 44(1):  20220607.  doi:10.7503/cjcu20220607

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Hollow mesoporous structures have great potential in catalysis， energy storage and conversion， biomedicine， etc.， due to their abundant inner void space and porous permeable shells. However， there is still a lack of efficient， simple and green synthesis methods. Herein， sodium citrate nanoparticles with excellent colloidal stability were used as templates for the direct growth of mesoporous silica shells through the interfacial co-assembly of cetyltrimethylammonium bromide（CTAB） micelles and hydrolyzed oligomer of tetraethyl orthosilicate（TEOS）. The hollow mesoporous structures were obtained simply after removal of the CTAB micelles and colloidal sodium citrate nanoparticles by ethanol and water washing. Further studies have shown that electrostatic interactions between negatively charged colloidal sodium citrate nanoparticles and CTAB micelles were key for the polymerization assembly of silicon oxide oligomer on the nanoparticle surface. More importantly， the morphology and shell thickness of hollow mesoporous structures could be accurately adjusted through the control of reaction time. Moreover， the hollow mesoporous structures could improve the mass transfer significantly， which can act as an ideal support for metal catalysts. As a proof of concept， the Au nanoparticles loaded hollow mesoporous silica nanospheres showed excellent catalytic activity for reduction of 4-nitrophenol. This work provided a new insight into the green and simple synthesis of hollow mesoporous materials.



Facile Synthesis of Metal/Carbon Electrocatalysts via Adsorption for Efficient Electrocatalytic Oxidation of HMF

LIU Zhichen, ZHANG Hongwei, ZHANG Bowen, CHEN Peng, YUAN Pei

2023, 44(1):  20220631.  doi:10.7503/cjcu20220631

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A simple adsorption method has been developed to prepare highly efficient electrocatalysts（Ni _x Fe_1‒x /HC） for 5-hydroxymethylfurfural（HMF） oxidation using mesoporous hollow carbon spheres（HC） as the carrier. X-ray diffraction（XRD）， field emission scanning electron microscopy（SEM）， X-ray photoelectron spectroscopy（XPS） and other characterizations were applied to characterize the phases， structural morphologies and electronic structures of the obtained Ni _x Fe_1‒x /HC catalysts. Linear sweep voltammetry， chronopotentiometry were used to evaluated the electrocatalytic activities of HMF oxidation of Ni _x Fe_1‒x /HC. The results show that the catalytic activity of Ni _x Fe_1‒x /HC catalysts increases first and then decreases with the increase of introduction amount of Fe. Among them， Ni_0.7Fe_0.3/HC show the best catalytic activity. The conversion of HMF is as high as 100%， the selectivity of 2，5-furandicarboxylic acid（FDCA） is 90.5%， and the Faradaic efficiency is 90.2%. Even after 10 cycles， the catalytic activity of Ni_0.7Fe_0.3/HC was only slightly reduced， exhibiting excellent catalytic stability.