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| 1 | 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 |
| 2 | Single‑Atom Catalysts:Advances and Challenges in Metal‑Support Interactions for Enhanced Electrocatalysis显示文摘Single-atom catalysts(SACs),which contain a single metal atom supported on a well-confined substrate,are among the most promising heterogeneous catalysts owing to their unique advantages,such as high intrinsic activity and selectivity,tunable bonds and coordination,abundant metal-containing active sites,and atomic economy.Since metal-support interactions(MSIs)in SACs exert a substantial influence on the catalytic properties,gaining a profound understanding and recognition of catalytic reactions depends greatly on investigating MSIs both experimentally and computationally.Hence,the engineer-ing and modulation of MSIs are regarded as one of the most efficient methods to rationally design SACs with disruptively enhanced catalytic properties.In this review,we track the recent advances in SACs from an MSI perspective.We then discuss the existing MSIs in SACs and elucidate the significant role of strong MSIs in catalytic properties and mechanisms.The chal-lenges hindering the rational design of supported SACs with strong MSIs,which are currently still far from being completely understood and overcome,are described.In addition,the correlation between strong MSIs and electrocatalytic activities in SACs,including an outlook to increase our understanding of MSIs,is discussed.Finally,the present review provides some perspectives and an in-depth understanding of strong MSIs to advance high-performing SACs. | Yang Mu Tingting Wang Jian Zhang Changgong Meng Yifu Zhang Zongkui Kou | 2022 | Electrochemical Energy Reviews2022，5，1： | 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 | Constructing a stable cobalt-nitrogen-carbon air cathode from coordinatively unsaturated zeolitic-imidazole frameworks for rechargeable zinc-air batteries显示文摘Zeolitic-imidazole frameworks(ZIFs)derivations have widely emerged as an efficient air cathode of zinc-air batteries(ZABs)due to excellent bifunctional oxygen electrocatalysis performance.However,they are not stable enough for long-term operation of rechargeable ZABs because of weak association with current collector,especially under bending conditions for flexible ZAB devices.Here,we show that by purposely designing coordinatively unsaturated ZIFs via a facile morphology regulation,which can be chemically linked on acid-treated carbon cloth,a stable Co-N-C air cathode is therefore derived where Co nanoparticles(NPs)are uniformly confined within the Co-N-C matrix on carbon cloth(Co/Co-N-C/CC).Specifically,when without being stabilized from carbon cloth,the pyrolysis of ZIFs with different unsaturated coordination levels has a negligible impact on the bifunctional oxygen-catalyzed performance.The optimal Co/Co-N-C/CC catalyst assembled ZAB possesses a large open circuit voltage of 1.415 V and a high peak power density of 163 mW·cm^(−2) as well as excellent cycling durability upon 630 discharge–charge cycles with 61%voltage efficiency remained,largely exceeding those of a benchmark Pt/C-IrO_(2) catalyst assembled ZAB.The synergy between Co NPs and active Co-N-C sites via electronic interaction induces the outstanding bifunctional oxygen-catalyzed activity and cathode performance.The present work highlights the importance of unsaturated coordination structures in ZIFs precursors for the performance of derived nanostructures in integrated electrodes. | Tingting Wang Meng Liu Somboon Chaemchuen Jichao Wang Ye Yuan Cheng Chen Ang Qiao Francis Verpoort Zongkui Kou | 2022 | Nano Research2022，15，7： | 0 |
| 5 | In situ constructing of ultrastable ceramic@graphene core-shell architectures as advanced metal catalyst supports toward oxygen reduction显示文摘The changeable structure of 2 D graphene nanosheets makes the Pt-based nanoparticles(NPs) possess a low efficiency toward oxygen reduction reaction(ORR) and a short lifetime for proton exchange membrane fuel cells. Thus, a unique Ti C@graphene core-shell structure material with low surface energy is designed and prepared by an in situ forming strategy, and firstly applied as a stable support of Pt NPs.The as-prepared Pt/GNS@Ti C catalyst presents a high activity. Especially, its ORR stability is remarkably improved. Even after 15000 potential cycles, the half-wave potential and mass activity toward ORR have almost no change. This can be attributed to that the graphene nanosheet existing in a sphere shape effectively avoids the restacking or folding caused by the giant surface tension in 2 D graphene nanosheets,impeding the decrease of the triple-phase boundary on Pt NPs. Significantly, the power density of fuel cells with our novel catalyst reaches 853 m V cm^(–2) under a low Pt loading(0.25 mg Pt cm^(–2)) and H_2/Air conditions. These indicate the new ceramic@graphene core-shell nanocomposite is a promising application in fuel cells and other fields. | HuiWu Tao Peng Zongkui Kou Kun Cheng Jie Zhang Jian Zhang Tian Meng Shichun Mu | 2017 | Journal of Energy Chemistry2017，26，6： | 0 |
| 6 | In-situ surface self-reconstruction in ternary transition metal dichalcogenide nanorod arrays enables efficient electrocatalytic oxygen evolution显示文摘Water splitting has received more and more attention because of its huge potential to generate clean and renewable energy.The highly active and durable oxygen evolution reaction(OER)catalysts play a decisive factor in achieving efficient water splitting.The identification of authentic active origin under the service conditions can prompt a more reasonable design of catalysts together with well-confined micro-/nano-structures to boost the efficiency of water splitting.Herein,Fe,Co,and Ni ternary transition metal dichalcogenide(FCND)nanorod arrays on Ni foam are purposely designed as an active and stable low-cost OER pre-catalyst for the electrolysis of water in alkaline media.The optimized FCND catalyst demonstrated a lower overpotential than the binary and unary counterparts,and a 27-fold rise in kinetic current density at the overpotential of 300 m V compared to the nickel dichalcogenide counterpart.Raman spectra and other structural characterizations at different potentials reveal that the in-situ surface self-reconstruction from FCND to ternary transition metal oxyhydroxides(FCNOH)on catalyst surfaces initiated at about 1.5 V,which is identified as the origin of OER activity.The surface selfreconstruction towards FCNOH also enables excellent stability,without fading upon the test for 50 h. | Qiang Chen Yulu Fu Jialun Jin Wenjie Zang Xiong Liu Xiangyong Zhang Wenzhong Huang Zongkui Kou John Wang Liang Zhou Liqiang Mai | 2021 | Journal of Energy Chemistry2021，30，4： | 0 |
| 7 | Single-atom metal-nitrogen-carbon catalysts energize single molecule detection for biosensing显示文摘Biosensors featuring single molecule detection present huge opportunities as well as challenges in food safety inspection,disease diagnosis,and environmental monitoring.Single-molecule detection is largely lacking of high enough activity,precision molecule selectivity,and understanding in the exact operating mechanism.Single-atom catalysts(SACs),especially those metals-nitrogen-carbon that mimic the natural metalloenzyme structure,and with well-defined metal atom bond configurations,high level of molecular selectivity,and easy fabrication,endow single molecule detections with practical-use feasibilities.The recent advances in single-atom catalysts also present new pathways in the key mechanism understandings.In this short review,we will first visit the brief history and advantages of SACs that have been explored only recently for molecule-scale biosensors,where they are analogous and also differentiated from those nanozymes and natural metalloenzymes.Their applications in electrochemical,photochemical,and photoelectrochemical sensors are then discussed comprehensively by focusing on the different molecule-scale sensing modes in achieving local coordination-modulated signal amplifications.Finally,we identify new opportunities and challenges faced by these SACs-based single molecule detections in the further development of biosensors. | Xianyang Zhang Pengfei Chen Siwuxie He Bowen Jiang Yong Wang Yonghua Cheng Jian Peng Francis Verpoort John Wang Zongkui Kou | 2023 | InfoMat2023，5，6： | 0 |
| 8 | Correlative Mn-Co catalyst excels Pt in oxygen reduction reaction of quasi-solid-state zinc-air batteries显示文摘Zn-air batteries(ZABs)as a class of promising energy storage setups are generally powered by efficient and robust catalysts at the oxygen-involving cathode.Although the existing non-noble catalysts have outperformed noble Pt benchmark in the alkaline liquid-state ZABs,to the best of our knowledge few have excelled Pt in quasi-solid-state(QSS)ZABs.Herein,we found that an integrated Mn-Co cathode derived from the bimetallic Mn/Co metal organic frameworks generates a 1.4-fold greater power density in the QSS ZABs than a Pt cathode while its power density in liquid-state ZABs is only 0.8-fold of the latter.Moreover,such Mn-Co catalyst delivers high-rate oxygen reduction reaction(ORR)capability with half-wave potential of 0.84 V.The in-depth characterizations and analyses have demonstrated that the Co and Mn species show the specific affinity towards H_(2)O and O_(2),respectively,synergizing the ORR process in the water-deficient environment of QSS ZABs.This work has enlightened the rational design of non-noble metal catalysts to improve the power density of QSS ZABs. | Tingting Wang Jincheng Huang Wei Sang Cai Zhou Bohan Zhang Wei Zhu Kang Du Zongkui Kou Shengxiang Wang | 2024 | Nano Research2024，17，5： | 0 |
| 9 | Fundamentals,On‑Going Advances and Challenges of Electrochemical Carbon Dioxide Reduction显示文摘Electrochemical carbon dioxide reduction(ECR)is an attractive pathway to synthesize useful fuels and chemical feedstocks,especially when paired with renewable electricity as the energy source.In this overview,we examine the recently witnessed advances and on-going pursuits of ECR in terms of the key fundamental mechanisms,basic experimentation principles,electrocatalysts and the electrochemical setup for ECR,aiming at offering timely key insights into solving the unsettled bottleneck issues.The reaction pathways are discussed in relation to the generation of single-,double-and multi-carbon products by the ECR,as well as the underlying principles in catalyst design to form them both efficiently and selectively.For the rational design of electrocatalysis,we look into the critically important roles played by various in situ and operando experimental techniques and computational simulations,where the key priorities are to engineer the highly active and selec-tive ECR catalysts for the specifically targeted products.Indeed,with the purposely designed high activity and selectivity,one would be able to“magically”transform a bottle of CO_(2)-riched“coke drink”to a glass of“beer”with the desired alcohol product in a layman term,instead of a bottle of formic acid.Nonetheless,there are still considerable complications and challenges ahead.As a dynamically rapid-advancing research frontier for both energy and the environment,there are great opportunities and obstacles in the ECR scale up. | Zongkui Kou Xin Li Tingting Wang Yuanyuan Ma Wenjie Zang Guangdi Nie John Wang | 2022 | Electrochemical Energy Reviews2022，5，1： | 0 |
| 10 | In situ confined vertical growth of Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)nanoarrays on rGO for an efficient oxygen evolution reaction显示文摘Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silicate hydroxide[Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)]is vertically grown on a reduced graphene oxide(rGO)support(CNS@rGO).This is developed as a low-cost and prospective OER catalyst.Compared to cobalt or nickel silicate hydroxide@rGO(CS@rGO and NS@rGO,respectively)nanoarrays,the bimetal CNS@rGO nanoarray exhibits impressive OER performance with an overpotential of 307 mV@10 mA cm^(-2).This value is higher than that of CS@rGO and NS@rGO.The CNS@rGO nanoarray has an overpotential of 446 mV@100 mA cm^(-2),about 1.4 times that of the commercial RuO_(2)electrocatalyst.The achieved OER activity is superior to the state-of-the-art metal oxides/hydroxides and their derivatives.The vertically grown nanostructure and optimized metal-support electronic interactions play an indispensable role for OER performance improvement,including a fast electron transfer pathway,short proton/electron diffusion distance,more active metal centers,as well as optimized dualatomic electron density.Taking advantage of interlay chemical regulation and the in-situ growth method,the advanced-structural CNS@rGO nanoarrays provide a new horizon to the rational and flexible design of efficient and promising OER electrocatalysts. | Yang Mu Xiaoyu Pei Yunfeng Zhao Xueying Dong Zongkui Kou Miao Cui Changgong Meng Yifu Zhang | 2023 | Nano Materials Science2023，5，4： | 0 |
| 11 | 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 |
| 12 | Well-structured 3D channels within GO-based membranes enable ultrafast wastewater treatment显示文摘Graphene oxide(GO)-based membranes have been widely studied for realizing efficient wastewater treatment,due to their easily functionalizeable surfaces and tunable interlayer structures.However,the irregular structure of water channels within GO-based membrane has largely confined water permeance and prevented the simultaneously improvement of purification performance.Herein,we purposely construct the well-structured three-dimensional(3D)water channels featuring regular and negatively-charged properties in the GO/SiO_(2)composite membrane via in situ close-packing assembly of SiO_(2)nanoparticles onto GO nanosheets.Such regular 3D channels can improve the water permeance to a record-high value of 33,431.5±559.9 L·m^(−2)·h−1(LMH)bar−1,which is several-fold higher than those of current state-of-the-art GO-based membranes.We further demonstrate that benefiting from negative charges on both GO and SiO2,these negatively-charged 3D channels enable the charge selectivity well toward dye in wastewater where the rejection for positive-charged and negative-charged dye molecules is 99.6%vs.7.2%,respectively.The 3D channels can also accelerate oil/water(O/W)separation process,in which the O/W permeance and oil rejection can reach 19,589.2±1,189.7 LMH bar−1 and 98.2%,respectively.The present work unveils the positive role of well-structured 3D channels on synchronizing the remarkable improvement of both water permeance and purification performance for highly efficient wastewater treatment. | Huaqiang Fu Zhe Wang Peng Li Wei Qian Zixin Zhang Xin Zhao Hao Feng Zhugen Yang Zongkui Kou Daping He | 2023 | Nano Research2023，16，2： | 0 |
| 13 | Vertically mounting molybdenum disulfide nanosheets on dimolybdenum carbide nanomeshes enables efficient hydrogen evolution显示文摘Designing hierarchical heterostructure to optimize the adsorption of hydrogen intermediate(H*)is impressive for hydrogen evolution reaction(HER)catalysis.Herein,we show that vertically mounting two-dimensional(2D)layered molybdenum disulfide(MoS_(2))nanosheets on 2D nonlayered dimolybdenum carbide(Mo_(2)C)nanomeshes to form a hierarchical heterostructure largely accelerates the HER kinetics in acidic electrolyte due to the weakening adsorption strength of H*on 2D Mo_(2)C nanomeshes.Our hierarchical MoS2/Mo2C heterostructure therefore gives a decrease of overpotential for up to 500 mV at-10 mA·cm^(-2)and an almost 200-fold higher kinetics current density compared with the pristine Mo2C nanomeshes and maintains robust stability with a small drop of overpotential for only 16 mV upon 5,000 cycles.We further rationalize this finding by theoretical calculations and find an optimized adsorption free energy of H*,identifying that the MoS_(2)featuring strong H*desorption plays a key role in weakening the strong binding of Mo_(2)C with H*and therefore improves the intrinsic HER activity on active C sites of Mo_(2)C.This present finding shines the light on the rational design of heterostructured catalysts with synergistic geometry. | Tingting Wang Pengyan Wang Yajun Pang Yitian Wu Jin Yang Hao Chen Xiaorui Gao Shichun Mu Zongkui Kou | 2022 | Nano Research2022，15，5： | 0 |
| 14 | Nanohollow Carbon for Rechargeable Batteries:Ongoing Progresses and Challenges显示文摘Among the various morphologies of carbon-based materials,hollow carbon nanostructures are of particular interest for energy storage.They have been widely investigated as electrode materials in different types of rechargeable batteries,owing to their high surface areas in association with the high surface-to-volume ratios,controllable pores and pore size distribution,high electrical conductivity,and excellent chemical and mechanical stability,which are beneficial for providing active sites,accelerating electrons/ions transfer,interacting with electrolytes,and giving rise to high specific capacity,rate capability,cycling ability,and overall electrochemical performance.In this overview,we look into the ongoing progresses that are being made with the nanohollow carbon materials,including nanospheres,nanopolyhedrons,and nanofibers,in relation to their applications in the main types of rechargeable batteries.The design and synthesis strategies for them and their electrochemical performance in rechargeable batteries,including lithium-ion batteries,sodium-ion batteries,potassium-ion batteries,and lithium–sulfur batteries are comprehensively reviewed and discussed,together with the challenges being faced and perspectives for them. | Jiangmin Jiang Guangdi Nie Ping Nie Zhiwei Li Zhenghui Pan Zongkui Kou Hui Dou Xiaogang Zhang John Wang | 2020 | Nano-Micro Letters2020，12，12： | 0 |
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