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| 1 | Defect and Doping Co‑Engineered Non‑Metal Nanocarbon ORR Electrocatalyst显示文摘Exploring low-cost and earth-abundant oxygen reduction reaction(ORR)electrocatalyst is essential for fuel cells and metal–air batteries.Among them,non-metal nanocarbon with multiple advantages of low cost,abundance,high conductivity,good durability,and competitive activity has attracted intense interest in recent years.The enhanced ORR activities of the nanocarbons are normally thought to originate from heteroatom(e.g.,N,B,P,or S)doping or various induced defects.However,in practice,carbon-based materials usually contain both dopants and defects.In this regard,in terms of the co-engineering of heteroatom doping and defect inducing,we present an overview of recent advances in developing non-metal carbon-based electrocatalysts for the ORR.The characteristics,ORR performance,and the related mechanism of these functionalized nanocarbons by heteroatom doping,defect inducing,and in particular their synergistic promotion effect are emphatically analyzed and discussed.Finally,the current issues and perspectives in developing carbon-based electrocatalysts from both of heteroatom doping and defect engineering are proposed.This review will be beneficial for the rational design and manufacturing of highly efficient carbon-based materials for electrocatalysis. | Jian Zhang Jingjing Zhang Feng He Yijun Chen Jiawei Zhu Deli Wang Shichun Mu Hui Ying Yang | 2021 | Nano-Micro Letters2021，13，4： | 8 |
| 2 | Nurturing the marriages of single atoms with atomic clusters and nanoparticles for better heterogeneous electrocatalysis显示文摘Single-atom catalysts,featuring some of the most unique activities,selectivity,and high metal utilization,have been extensively studied over the past decade.Given their high activity,selectivity,especially towards small molecules or key intermediate conversions,they can be synergized together with other active species(typically other single atoms,atomic clusters,or nanoparticles)in either tandem or parallel or both,leading to much better performance in complex catalytic processes.Although there have been reports on effectively combining the multiple components into one single catalytic entity,the combination and synergy between single atoms and other active species have not been reviewed and examined in a systematic manner.Herein,in this overview,the key synergistic interactions,binary complementary effects,and the bifunctional functions of single atoms with other active species are defined and discussed in detail.The integration functions of their marriages are in-vestigated with particular emphasis on the homogeneous and heterogeneous combinations,spatial distribution,synthetic strategies,and the thus-derived outstanding catalytic performance,together with new light shined on the catalytic mechanisms by zooming in several case studies.The dynamic nature of each of the active species and in particular their interactions in such new catalytic entities in the heterogeneous electrocatalytic processes are visited,on the basis of the in situ/operando evidence.Last,we feature the current chal-lenges and future perspectives of these integrated catalytic entities that can offer guidance for advanced catalyst design by the rational combination and synergy of binary or multiple active species. | Lei Zhang Jiawei Zhu Xin Li Shichun Mu Francis Verpoort Junmin Xue Zongkui Kou John Wang | 2022 | Interdisciplinary Materials2022，1，1： | 3 |
| 3 | Tunable Ru-Ru2P heterostructures with charge redistribution for efficient pH-universal hydrogen evolution显示文摘Designing synergistic heterogeneous catalytic interfaces is the key to developing highly compatible pH-universal electrocatalysts for complex chemical environments.Our theoretical calculation results demonstrate that the Ru-Ru2P heterointerface can not only promote the redistribution of charges,but also reduce the d-band center,and then enhances the adsorption capacity of the key intermediate.However,in situ and facile synthesis of Ru-Ru2P heterostructures is severely limited by thermodynamic obstacles.Herein,we propose a molten salt-assisted catalytic synthesis scheme,and successfully build a series of homologous metallic Ru-Ru2P heterostructure catalysts with different molar ratios of Ru to P under atmospheric pressure and low-temperature(400C).The resultant Ru-Ru2P with rich heterostructures show the Pt-like HER performance in different pH media.Particularly,it is prominent under alkaline conditions(18 mV@10 mA cm^(2)),which outperforms the Pt catalyst(37 mV@10 mA cm^(2)).Furthermore,Ru-Ru2P heterostructures also show certain potential in the electrolysis of seawater to produce hydrogen.This work represents a significant supplement of high-efficiency pH-universal HER catalysts,and provides a new light on interface engineering in energy technology fields and beyond. | Ding Chen Ruohan Yu Ruihu Lu Zonghua Pu Pengyan Wang Jiawei Zhu Pengxia Ji Dulan Wu Jinsong Wu Yan Zhao Zongkui Kou Jun Yu Shichun Mu | 2022 | InfoMat2022，4，5： | 2 |
| 4 | Ultra-small platinum nanoparticles segregated by nickle sites for efficient ORR and HER processes显示文摘In the electrochemical process,Pt nanoparticles(NPs)in Pt-based catalysts usually agglomerate due to Oswald ripening or lack of restraint,ultimately resulting in reduction of the active sites and catalytic efficiency.How to uniformly disperse and firmly fix Pt NPs on carbon matrix with suitable particle size for catalysis is still a big challenge.Herein,to prevent the agglomeration and shedding of Pt NPs,Ni species is introduced and are evenly dispersed in the surface of carbon matrix in the form of Ni-N-C active sites(Ni ZIF-NC).The Ni sites can be used to anchor Pt NPs,and then effectively limit the further growth and agglomeration of Pt NPs during the reaction process.Compared with commercial Pt/C catalyst,Pt@Ni ZIF-NC,with ultralow Pt loading(7 wt%)and ideal particle size(2.3 nm),not only increases the active center,but also promotes the catalysis kinetics,greatly improving the ORR and HER catalytic activity.Under acidic conditions,its half-wave potential(0.902 V)is superior to commercial Pt/C(0.861 V),and the mass activity(0.38 A per mg Pt)at 0.9 V is 4.7 times that of Pt/C(0.08 A per mg Pt).Besides,it also shows outstanding HER performance.At 20 and 30 mV,its mass activity is even 2 and 6 times that of Pt/C,respectively.Whether it is under ORR or HER conditions,it still shows excellent durability.These undoubtedly indicate the realization of dual-functional catalysts with low-Pt and high-efficiency properties. | Lvhan Liang Huihui jin Huang Zhou Bingshuai Liu Chenxi Hu Ding Chen Jiawei Zhu Zhe Wang Hai-Wen Li Suli Liu Daping He Shichun Mu | 2022 | Journal of Energy Chemistry2022，31，2： | 2 |
| 5 | Epitaxially Grown Ru Clusters-Nickel Nitride Heterostructure Advances Water Electrolysis Kinetics in Alkaline and Seawater Media显示文摘The epitaxial heterostructure can be rationally designed based on the in situ growth of two compatible phases with lattice similarity,in which the modulated electronic states and tuned adsorption behaviors are conducive to the enhancement of electrocatalytic activity.Herein,theoretical simulations first disclose the charge transfer trend and reinforced inherent electron conduction around the epitaxial heterointerface between Ru clusters and Ni_(3)N substrate(cRu-Ni_(3)N),thus leading to the optimized adsorption behaviors and reduced activation energy barriers.Subsequently,the defectrich nanosheets with the epitaxially grown cRu-Ni_(3)N heterointerface are successfully constructed.Impressively,by virtue of the superiority of intrinsic activity and reaction kinetics,such unique epitaxial heterostructure exhibits remarkable bifunctional catalytic activity toward electrocatalytic OER(226 mV@20 mA cm^(−2))and HER(32 mV@10 mA cm^(−2))in alkaline media.Furthermore,it also shows great application prospect in alkaline freshwater and seawater splitting,as well as solar-to-hydrogen integrated system.This work could provide beneficial enlightenment for the establishment of advanced electrocatalysts with epitaxial heterointerfaces. | Jiawei Zhu Ruihu Lu Wenjie Shi Lei Gong Ding Chen Pengyan Wang Lei Chen Jinsong Wu Shichun Mu Yan Zhao | 2023 | Energy & Environmental Materials2023，6，2： | 2 |
| 6 | In situ generated layered NiFe-LDH/MOF heterostructure nanosheet arrays with abundant defects for efficient alkaline and seawater oxidation显示文摘As the main limiting step of overall water splitting,oxygen evolution reaction(OER)is urgent to be enhanced by developing efficient catalysts to promote the process of electrolytic water.Based on theoretical analysis,the Ni-metal-organic framework(Ni-MOF)and NiFe-layered double hydroxide(NiFe-LDH)(NiFe-LDH/MOF)heterostructure can optimize the energy barrier of the OER process and decrease the adsorption energy of oxygen-containing intermediates,effectively accelerating the OER kinetics.Accordingly,layered NiFe-LDH/MOF heterostructures are in situ constructed through a facile two-step reaction process,with substantial oxygen defects and lattice defects that further improve the catalytic performance.As a result,only 208 and 275 mV OER overpotentials are needed for NiFe-LDH/MOF to drive the current densities of 20 and 100 mA·cm^(-2)in 1 M KOH solutions,and even maintain catalytic stability of 100 h at 20 mA·cm^(-2).When applied to seawater oxidation,only 235 and 307 mV OER overpotentials are required to achieve the current densities of 20 and 100 mA·cm^(-2),respectively,with almost no attenuation for 100 h stability test at 20 mA·cm^(-2),all better than commercial RuO_(2).This work provides the theoretical and experimental basis and a new idea for efficiently driving fresh water and seawater cracking by heterostructure and defect coupling design toward catalysts. | Manjie Xiao Can Wu Jiawei Zhu Chengtian Zhang Yan Li Jiahui Lyu Weihao Zeng Haiwen Li Lei Chen Shichun Mu | 2023 | Nano Research2023，16，7： | 1 |
| 7 | Real-time retrieval of submicron aerosol size distributions from multi-wavelength spectral extinction measurements显示文摘The real-time retrieval of submicron aerosol size distributions is of major interest for applications. Based on the Mie theory,the spectral extinction method offers a simple measurement principle and a convenient optical arrangement. In contrast to the relative simplicity of the experimental measurement the retrieval of the particles size distribution and particle concentration from the spectral extinction method is difficult. Mie scattering Equation is a Fredholm Integral Equation of the First Kind. This paper develops a hybrid iterative model-dependent algorithm for on-line particle sizing from extinction spectra which is both computationally efficient and accurate. Applying the refined Mie diagnostic iterative procedures within some candidate solutions can identify the unique result accurately and rapidly enough for real time measurement. With the addition of added Gaussian noise,an average tolerance up to 5% of noise level is kept for particle size from submicron to micrometer under moderate polydispersity. | CHEN Jiawei YANG Mu FENG Haibao NI Qijun | 2016 | Instrumentation2016，3，1： | 1 |
| 8 | A new strategy to access Co/N co-doped carbon nanotubes as oxygen reduction reaction catalysts显示文摘Carbon nanotubes(CNTs),as one-dimensional nanomaterials,show great potential in energy conversion and storage due to their efficient electrical conductivity and mass transfer.However,the security risks,time-consuming and high cost of the preparation process hinder its further application.Here,we develop that a negative pressure rather than a following gas environment can promote the generation of cobalt and nitrogen co-doped CNTs(Co/N-CNTs) by using cobalt zeolitic imidazolate framework(ZIF-67) as a precursor,in which the negative pressure plays a key role in adjusting the size of cobalt nanoparticles and stimulating the rearragement of carbon atoms for forming CNTs.Importantly,the obtained Co/N-CNTs,with high content of pyridinic nitrogen and abundant graphitized structure,exhibit superior catalytic activity for oxygen reduction reaction(ORR) with half-wave potential(E_(1/2)) of 0.85 V and durability in terms of the minimum current loss(2%) after the 30,000 s test.Our development provides a new pathway for large-scale and cost-effective preparation of metal-doped CNTs for various applications. | Bingshuai Liu Huang Zhou Huihui Jin Jiawei Zhu Zhe Wang Chenxi Hu Lvhan Liang Shichun Mu Daping He | 2021 | Chinese Chemical Letters2021，32，1： | 1 |
| 9 | Propelling polysulfide redox by Fe_(3)C-FeN heterostructure@nitrogendoped carbon framework towards high-efficiency Li-S batteries显示文摘Lithium-sulfur(Li-S) batteries hold great promise in next-generation high-energy-density energy storage systems,but the intractable shuttle effect and the sluggish redox kinetics of polysulfides hinder the practical implementation of Li-S batteries.Here,heterostructured Fe_(3)C-FeN nanoparticles dotted in the threedimensional-ordered nitrogen-doped carbon framework(Fe_(3)C-FeN@NCF) were synthesized by molecular engineering combined with heterointerface engineering,and were applied to regulate the immobilization-diffusion-conversion behavior of polar polysulfides.It is experimentally and theoretically demonstrated that the heterointerface between Fe_(3)C and FeN exhibits high sulfiphilicity and high electronic/ionic conductivity,thus effectively capturing polysulfides and accelerating the bidirectional conversion of sulfur species.Meanwhile,the holey carbon framework functions as the scaffold to highly disperse binary nanoparticles,ensuring the sufficient exposure of active sites and the easy accessibility for lithium ions and electrons.By virtue of these synergistic merits,the Li-S batteries based on Fe_(3)CFeN@NCF-modified separators afford excellent electrochemical performances including a high rate capacity of 858 mA h g^(-1)at 2 C and a low capacity decay rate of 0.07% per cycle after 800 cycles at 1C This work provides inspiration for the design of heterostructured compounds and sheds light on the potential of heterostructure in high-efficiency Li-S batteries. | Mengdi Zhang Jiawei Mu Yanan Li Yuanyuan Pan Zhiliang Dong Bei Chen Shiwei Guo Wenhan Yuan Haiqiu Fang Han Hu Mingbo Wu | 2023 | Journal of Energy Chemistry2023，，3： | 1 |
| 10 | Tuning Active Metal Atomic Spacing by Filling of Light Atoms and Resulting Reversed Hydrogen Adsorption-Distance Relationship for Efficient Catalysis显示文摘Precisely tuning the spacing of the active centers on the atomic scale is of great significance to improve the catalytic activity and deepen the understanding of the catalytic mechanism,but still remains a challenge.Here,we develop a strategy to dilute catalytically active metal interatomic spacing(d_(M-M))with light atoms and discover the unusual adsorption patterns.For example,by elevating the content of boron as interstitial atoms,the atomic spacing of osmium(d_(Os-Os))gradually increases from 2.73 to 2.96?.More importantly,we find that,with the increase in dOs-Os,the hydrogen adsorption-distance relationship is reversed via downshifting d-band states,which breaks the traditional cognition,thereby optimizing the H adsorption and H_2O dissociation on the electrode surface during the catalytic process;this finally leads to a nearly linear increase in hydrogen evolution reaction activity.Namely,the maximum dOs-Os of 2.96?presents the optimal HER activity(8 mV@10 mA cm^(-2))in alkaline media as well as suppressed O adsorption and thus promoted stability.It is believed that this novel atomic-level distance modulation strategy of catalytic sites and the reversed hydrogen adsorption-distance relationship can shew new insights for optimal design of highly efficient catalysts. | Ding Chen Ruihu Lu Ruohan Yu Hongyu Zhao Dulan Wu Youtao Yao Kesong Yu Jiawei Zhu Pengxia Ji Zonghua Pu Zongkui Kou Jun Yu Jinsong Wu Shichun Mu | 2023 | Nano-Micro Letters2023，15，10： | 0 |
| 11 | Laser irradiation constructing all-in-one defective graphenepolyimide separator for effective restraint of lithium dendrites and shuttle effect显示文摘The commercialization of lithium-sulfur(Li-S)batteries faces several bottlenecks,and the major two of which are the shuttle effect of polysulfides and the wild growth of Li dendrites,responsible for fast capacity decay and severe safety issues.As an essential component of Li-S batteries,the structure and properties of the separators are closely related to the above problems,and the exploration of multifunctional separators is highly sought-after.Herein,an integrated separator composited of defective graphene and polyimide(DG-PI)was innovatively fabricated by electrospinning combined with the laser-induced carbonization strategy.The all-in-one compact architecture with well-interconnected channels shows superior mechanical and thermal stability and wettability.More importantly,the PI nanofibers containing N–/O–functional groups can induce the uniform deposition of lithium on the anode surface,while the DG framework with abundant pentagonal/heptagonal rings and vacancies can strongly trap polysulfides and accelerate polysulfide transformation on the cathode side.The strong chemical interaction between the insulative PI layer and the conductive DG layer modulates the surface charge distribution of each other,leading to more prominent contributions to restraining lithium dendrites and shuttle effect.Therefore,the Li-S batteries based on the integrated DG-PI separators afford an excellent performance in protecting lithium anode(stable cycles of 200 h at 5 mA·cm^(−2))and good cycling stability with a low capacity decay of 0.05%per cycle after 700 cycles at 1 C.This work offers a new design concept of multifunctional Li-S battery separators and broadens the application scope of laser micro-nano fabrication technology. | Jiawei Mu Mengdi Zhang Yanan Li Zhiliang Dong Yuanyuan Pan Bei Chen Zhengqiu He Haiqiu Fang Shuoshuo Kong Xin Gu Han Hu Mingbo Wu | 2023 | Nano Research2023，16，10： | 0 |
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