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Nano Research 2022年第10期15卷 8804-8809页

作者： Mingju Lu Jialu Wang Guoyuan Ren Fengjuan Qin Zhiqiang Zhao Kai Li Wenxing Chen Yuqing Lin Department of Chemistry Capital Normal UniversityBeijing 100048China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China

Although nanozyme has become an emerging area of research attracting extensive attention recently,the activity and specificity of currently reported nanozymes are generally lower than those of natural enzymes.Developing highly active and specific nanozymes is therefore extremely necessary and also remains a great challenge.Superoxide dismutase(SOD)catalyzes the disproportionation of cytotoxic O_(2)·^(−)into hydrogen peroxide and oxygen,and plays an important role in reducing human oxidative stress.In this work,we prepare Cu single-atom catalysts(Cu/GO SACs,GO=graphene oxide)through a simple and low-cost strategy at room temperature using Cu foam and graphene oxide.Cu/GO SACs can maintain excellent catalytic activity under harsh environment.Compared with the natural enzyme,SOD-like Cu/GO SAC nanozyme has higher catalytic activity and meanwhile,it does not possess the common properties of other mimic enzymes often existing in nanomaterials.Based on the excellent SOD-like enzyme activity of Cu/GO SACs,it successfully eliminates the active oxygen in cigarette smoke.This work not only provides a new idea for the design and synthesis of nanozymes with excellent SOD mimetic properties,but also is promising in the treatment of lung injury and inflammatory diseases related to free radical production.

关键词： Cu/graphene oxide(GO)single-atom catalysts(SACs) superoxide dismutase(SOD)-like activity activity specificity superoxide free radicals

Single atom catalysts by atomic diffusion strategy

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Nano Research 2021年第12期14卷 4398-4416页

作者： Lihong Lin Zhuo Chen Wenxing Chen Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing100081China

The depletion of energy and increasing environmental pressure have become one of the main challenges in the world today.Synthetic high-efficiency catalysts bring hope for efficient conversion of energy and effective treatment of pollutants,especially,single-atom catalysts(SACs)are promising candidates.Herein,we comprehensively summarizes the atomic diffusion strategy,which is considered as an effective method to prepare a series of SACs.According to the different diffusion forms of the precursors,we review the synthesis pathways of SACs from three aspects:gas diffusion,solid diffusion and liquid diffusion.The gaseous diffusion method mainly discusses atomic layer deposition(ALD)and chemical vapor deposition(CVD),both of which carry out gas phase mass transfer at high temperatures.The solid-state diffusion method can be divided into nanoparticle transformation into single atoms and solid atom migration.Liquid diffusion mainly describes the electrochemical method and the molten salt method.We hope this review can trigger the rational design of SACs.

关键词： single atomic catalyst gas diffusion solid diffusion liquid diffusion

Interfacial engineering of 3D hollow CoSe_(2)@ultrathin MoSe_(2)core@shell heterostructure for efficient pH-universal hydrogen evolution reaction

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Nano Research 2022年第4期15卷 2895-2904页

作者： Lili Zhang Yuanting Lei Danni Zhou Chengli Xiong Zhuoli Jiang Xinyuan Li Huishan Shang Yafei Zhao Wenxing Chen Bing Zhang School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Department of Chemistry Tsinghua UniversityBeijing 100084China

Rational design and construction of low-cost and highly efficient electrocatalysts for hydrogen evolution reaction(HER)is meaningful but challenging.Herein,a robust three dimensional(3D)hollow CoSe_(2)@ultrathin MoSe_(2)core@shell heterostructure(CoSe_(2)@MoSe_(2))is proposed as an efficient HER electrocatalyst through interfacial engineering.Benefitting from the abundant heterogeneous interfaces on CoSe_(2)@MoSe_(2),the exposed edge active sites are maximized and the charge transfer at the hetero-interfaces is accelerated,thus facilitating the HER kinetics.It exhibits remarkable performance in pH-universal conditions.Notably,it only needs an overpotential(η10)of 108 mV to reach a current density of 10 mA·cm^(-2)in 1.0 M KOH,outperforming most of the reported transition metal selenides electrocatalysts.Density functional theory(DFT)calculations unveil that the heterointerfaces synergistically optimize the Gibbs free energies of H2O and H^(*)during alkaline HER,accelerating the reaction kinetics.The present work may provide new construction guidance for rational design of high-efficient electrocatalysts.

关键词： transition metal selenides hydrogen evolution reaction core@shell heterostructure pH-universal

Carbon-supported high-entropy Co-Zn-Cd-Cu-Mn sulfide nanoarrays promise high-performance overall water splitting

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Nano Research 2022年第7期15卷 6054-6061页

作者： Yuanting Lei Lili Zhang Wenjing Xu Chengli Xiong Wenxing Chen Xu Xiang Bing Zhang Huishan Shang School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

Transition metal sulfides with homogeneous multi-metallic elements promise high catalytic performance for water electrolysis owing to the unique structure and highly tailorable electrochemical property.Most existing synthetic routes require high temperature to ensure the uniform mixing of various elements,making the synthesis highly challenging.Here,for the first-time novel carbon fiber supported high-entropy Co-Zn-Cd-Cu-Mn sulfide(CoZnCdCuMnS@CF)nanoarrays are fabricated by the mild cation exchange strategy.Benefiting from the synergistic effect among multiple metals and the strong interfacial bonding between high-entropy Co-Zn-Cd-Cu-Mn sulfide nanoarrays and the carbon fiber support,CoZnCdCuMnS@CF exhibits superior catalytic activity and stability toward overall water splitting in alkaline medium.Impressively,CoZnCdCuMnS@CF only needs low overpotentials of 173 and 220 mV to reach the current density of 10 mA•cm^(−2),with excellent durability for over 70 and 113 h for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)respectively.More importantly,the bifunctional electrode(CoZnCdCuMnS@CF||CoZnCdCuMnS@CF)for overall water splitting can deliver a small cell voltage of 1.63 V to afford 10 mA•cm^(−2) and exhibit outstanding stability of negligible decay after 73 h continuous operation.This work provides a viable synthesis route toward advanced high-entropy materials with great potential applications.

关键词： electrocatalysis high-entropy metal sulfides oxygen evolution reaction hydrogen evolution reaction low-temperature cation exchange

Dimensional heterojunction design:The rising star of 2D bismuthbased nanostructured photocatalysts for solar-to-chemical conversion

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Nano Research 2023年第4期16卷 4310-4364页

作者： Joel Jie Foo Sue-Faye Ng Wee-Jun Ong School of energy and Chemical Engineering Xiamen University MalaysiaSelangor Darul Ehsan 43900Malaysia center of Excellence for NaNo energy&catalysis Technology(CONNECT) Xiamen University MalaysiaSelangor Darul Ehsan 43900Malaysia College of Chemistry and Chemical Engineering Xiamen UniversityXiamen 361005China Shenzhen Research Institute of Xiamen University Shenzhen 518057China

With the fast-pace digitalization evolution in the current generation’s lifestyle and the industry revolution,the energy demand has been skyrocketed.Recently,the two-dimensional(2D)bismuth-based nanomaterials emerged as a promising photocatalyst candidate in solar fuel conversion,not only for its exceptional light absorption capability and tunable optical properties,but it also can be synthesized into diverse variety of nanomaterials with different ranges of potential gap and band position to fulfill the potential requirement of wide range of photocatalytic reaction.Yet,the weak light harvesting ability and ultrafast charge recombination has restricted its potential in commercial application.Thus,recent researches have been focusing on tackling these issues by incorporating some modification strategies such as heteroatom doping,vacancy engineering,facet engineering,bismuth rich strategy and heterojunction engineering.Herein,this review article presents the state-of-the-art modifications on 2D bismuth-based parent material,specifically on the relationship between each of the modification strategy on the electronic properties and surface chemistry in achieving boosted photocatalytic performance.In the view of the unique charge interaction between two semiconductors with different dimensions,we systematically discuss the rational heterostructure design from the dimensionality perspective,namely,point-to-face,line-to-face,face-to-face,and bulk-to-face in solar fuel conversion to provide inspiring insights for future interface engineering.Finally,the challenges and the future research outlook in the solar-to-fuel conversion are highlighted to push forward the design of high-performance bismuth-based photocatalyst in realizing commercialscale solar-to-fuel conversion.

关键词： 2D heterojunction 2D nanomaterial CO_(2)reduction water splitting N2 fixation Z-scheme

In situ decorating the surface and interlayer of montmorillonite with Co_(0.5)Ni_(0.5)Fe_(2)O_(4) nanoparticles: A sustainable, biocompatible colorimetric platform for H_(2)O_(2) and acetylcholine

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Nano Research 2022年第10期15卷 9319-9326页

作者： Xixi Zhu Hongyu Li Tao Wu Hui Zhao Kaili Wu Wenjing Xu Fengjuan Qin Wenxing Chen Jinlong Zheng Qingyun Liu College of Chemical and Biological Engineering Shandong University of Science and TechnologyQingdao 266590China Beijing Advanced Innovation center for Materials Genome Engineering Shunde Graduate SchoolSchool of Mathematics and PhysicsUniversity of Science and Technology BeijingBeijing 100083China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China

Originated from nature and used for nature is a way of sustainable development.In this work,montmorillonite(MMT),a natural two-dimensional(2D)layered mineral,the surface and interlayer of which were nano-decorated by chemical synthesis technique was applied in biological detection field.Magnetic ferrite(Co_(0.5)Ni_(0.5)Fe_(2)O_(4))was anchored on the surface and intercalated in the interlayer of montmorillonite,which served as a competitive candidate of enzyme mimics.Cytotoxicity test toward HUVEC and Hela cells verified the good biocompatibility of Co_(0.5)Ni_(0.5)Fe_(2)O_(4)-MMT,guaranteeing its safety in biological applications.Based on the peroxidase-like activity of Co_(0.5)Ni_(0.5)Fe_(2)O_(4)-MMT,a colorimetric sensing platform for H_(2)O_(2) was established by a facile mix-anddetect approach with the detection limit of 0.565μM(3σ/slope).It was implied that the peroxidase-like activity of Co_(0.5)Ni_(0.5)Fe_(2)O_(4)-MMT was originated from generation of·OH and·O_(2)–produced from catalytic decomposition process of H_(2)O_(2).Coupled with cascaded catalytic reactions of ACh,a facile and efficient sensing platform for ACh with satisfactory anti-interference ability was established.Thus,all these remarkable features highlighted the superiority of Co_(0.5)Ni_(0.5)Fe_(2)O_(4)-MMT,and endowed it with a powerful competitiveness in the fields of environmental assessing,biosensing,and disease monitoring.

关键词： montmorillonite colorimetric assays hydrogen peroxide peroxidase-like activity nanozymes

The atomic interface effect of single atom catalysts for electrochemical hydrogen peroxide production

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Nano Research 2023年第8期16卷 10724-10741页

作者： Kaiyuan Liu Pengwan Chen Zhiyi Sun Wenxing Chen Qiang Zhou Xin Gao State Key Laboratory of Explosion Science and Technology Beijing Institute of TechnologyBeijing 100081China Advanced Technology Research Institute Beijing Institute of TechnologyJinan 250307China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China China Academy of Ordnance Science Beijing 100089China

Producing hydrogen peroxide(H_(2)O_(2))through an electrochemical oxygen reduction reaction(ORR)is a safe,green strategy and a promising alternative to traditional energy-intensive anthraquinone processes.Air and renewable power could be utilized for onsite and decentralized H_(2)O_(2)production,demonstrating significant application potential.Currently,single atom catalysts(SACs)have demonstrated significant advantages in the catalytic production of H_(2)O_(2)in 2e−ORR.However,the selectivity of SACs in ORR once puzzled researchers.This article reviews the research on the development and achievements of H_(2)O_(2)production by SACs catalysis in recent years.Especially,the structure-performance relationship is a guide to designing new SACs.Combining advanced characterization techniques and theoretical calculation methods,researchers have a clearer and more thorough understanding of the impact of the atomic interface of SACs on ORR catalytic performance.The coordination moiety formed between the active metal center atom and the support seriously determines the selectivity of SACs,mainly manifested in the adsorption of*OOH intermediates.Particularly,the atomic interface of metal atoms together with O/N co-coordination exhibit high selectivity and mass activity,and heteroatoms or functional groups on carbon supports present synergistic effects to promote the production of H_(2)O_(2)in 2e−ORR.Fine and accurate regulation of the atomic interface of SACs directly affects the 2e−ORR performance of the catalysts.Therefore,it is important to deeply understand the atomic interface of SACs and contribute to the development of novel catalysts.

关键词： single atom catalysts(SACs) atomic interface effect hydrogen peroxide(H_(2)O_(2))production electrochemical catalysis

Atomically Dispersed Dual‑Metal Sites Showing Unique Reactivity and Dynamism for Electrocatalysis

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Nano-Micro Letters 2023年第8期15卷 192-204页

作者： Jun‑Xi Wu Wen‑Xing Chen Chun‑Ting He Kai Zheng Lin‑Ling Zhuo Zhen‑Hua Zhao Jie‑Peng Zhang MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of ChemistrySun Yat-Sen UniversityGuangzhou 510275People’s Republic of China Key Lab of Fluorine and Silicon for energy Materials and Chemistry of Ministry of Education College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang 330022People’s Republic of China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081People’s Republic of China

The real structure and in situ evolution of catalysts under working conditions are of paramount importance,especially for bifunctional electrocatalysis.Here,we report asymmetric structural evolution and dynamic hydrogen-bonding promotion mechanism of an atomically dispersed electrocatalyst.Pyrolysis of Co/Ni-doped MAF-4/ZIF-8 yielded nitrogen-doped porous carbons functionalized by atomically dispersed Co–Ni dual-metal sites with an unprecedented N8V4 structure,which can serve as an efficient bifunctional electrocatalyst for overall water splitting.More importantly,the electrocatalyst showed remarkable activation behavior due to the in situ oxidation of the carbon substrate to form C–OH groups.Density functional theory calculations suggested that the flexible C–OH groups can form reversible hydrogen bonds with the oxygen evolution reaction intermediates,giving a bridge between elementary reactions to break the conventional scaling relationship.

关键词： Metal-organic frameworks Atomically dispersed catalyst Hydrogen bond Overall water splitting

Solar-powered chemistry: Engineering low-dimensional carbon nitride-based nanostructures for selective CO_(2) conversion to C_(1)- C_(2) products

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InfoMat 2022年第1期4卷 40-104页

作者： Sue-Faye Ng Joel Jie Foo Wee-Jun Ong School of energy and Chemical Engineering Xiamen University MalaysiaSepangSelangorMalaysia center of Excellence for NaNo energy&catalysis Technology(CONNECT) Xiamen University MalaysiaSepangSelangorMalaysia College of Chemistry and Chemical Engineering Xiamen UniversityXiamenChina

CO_(2)capture and conversion has been prospected as an auspicious technology to simultaneously tackle the rise in global CO_(2)emission and produce valueadded fuels with the goal of accomplishing carbon neutrality.A sustainable route to achieve this is via the utilization of solar energy,thereby harnessing the abundant and nonexhaustive resource to shift our reliance away from rapidly depleting fossil fuels.Graphitic carbon nitride(g-C_(3)N_(4))and its allotrope have earned its rank as a fascinating metal-free photocatalyst due to its superior stability,high surface-area-to-volume ratio,and tunable surface engineering.By leveraging these properties,robust carbon nitride-based nanostructures are engineered for photocatalytic CO_(2)conversion to energy-rich C_(1)-C_(2) product,which is indispensable in the chemical industry.Thus,this review presents the latest panorama of experimental and computational research on tuning the local electronic,surface chemical coordination environment,charge dynamics and optical properties of low-dimensional carbon nitride and its allotropes toward highly selective and efficient CO_(2)photoconversion.To name a few,structural engineering,point-defect engineering,heterojunction construction,and cocatalyst loading.To advance this frontier,critical insights are elucidated to establish the structure-performance relationship and unravel primary factors dictating the selectivity of C_(1)-C_(2) molecules from CO_(2)reduction.External-field assisted photocatalysis such as with electric(photoelectro-)and heat(photothermal)is discussed to uncover the synergistic contributions that drive the development in photochemistry.Last,future challenges and prospects are outlined for the potential application of solar-driven CO_(2)conversion,along with the scale-up strategy from the economic viewpoint toward the rational development of high-efficiency carbon nitride catalysts.

关键词： carbon nitride CO_(2)reduction external fields interfacial design nanostructure photocatalysis

Highly efficient hydrogen production from methanol by single nickel atoms anchored on defective boron nitride nanosheet

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Nano Research 2023年第7期16卷 8800-8808页

作者： Shengshu Yang Fang Zhang Haifa Qiu Ming Yang Fengjuan Qin Hao Tang Wenxing Chen Zhengang Liu Research center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China National Engineering Laboratory for VOCs Pollution Control Material&Technology University of Chinese Academy of SciencesBeijing 101408China Analytical and Testing center Beijing Institute of TechnologyBeijing 100081China Department of Applied Physics the Hong Kong Polytechnic UniversityHong Kong 999077China Energy&Catalysis Center School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China

Exploiting inexpensive and effective nickel-based catalysts that produce hydrogen from liquid organic hydrogen carriers(LOHCs)is crucial to alleviating the global energy and environmental crisis.In this study,we report a rational strategy that can realize atomically dispersed Ni atoms anchored on vacancy-abundant boron nitride nanosheets(Ni1/h-BNNS)with high specific surface area(up to 622 m^(2)·g^(-1))and abundant hydroxyl groups for high efficient hydrogen production.Methanol dehydrogenation results show an excellent hydrogen production performance catalyzed by this Ni1/h-BNNS,as evidenced by a remarkably high H_(2) yield rate(1684.23 mol·mol_(Ni)^(-1)·h^(-1)),nearly 100%selectivity toward hydrogen and CO,and high anti-coking performance.Density functional theory(DFT)calculations reveal that the outstanding catalytic performance of Ni1/h-BNNS primarily originates from the unique coordinated environment of atomically dispersed Ni(Ni-B_(2)O_(2))and the synergistic interaction between Ni single atoms and the h-BNNS support.Specifically,the coordinated O atoms play a decisive role in promoting the activity of Ni,and the neighboring B sites significantly decrease the energy barriers for the adsorption of key intermediates of methanol dehydrogenation.This study offers a novel strategy for developing high-performance and stable single-atom Ni catalysts by precisely controlling single-atom sites on h-BN support for sustainable hydrogen production.

关键词： single-atom catalyst coordination environment boron nitride hydrogen production liquid organic hydrogen carriers