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Crystal defect engineering of Bi_(2)Te_(3)nanosheets by Ce doping for efficient electrocatalytic nitrogen reduction

Nano Research 2023年第5期16卷 6544-6551页

作者： Jianli Nan Yongqin Liu Daiyong Chao Youxing Fang shaojun dong College of Chemistry Jilin UniversityChangchun 130012China Changchun State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China

Electrochemical nitrogen reduction reaction(NRR)is a promising method for the synthesis of ammonia(NH3).However,the electrochemical NRR process remains a great challenge in achieving a high NH3 yield rate and a high Faradaic efficiency(FE)due to the extremely strong N≡N bonds and the competing hydrogen evolution reaction(HER).Recently,bismuth telluride(Bi_(2)Te_(3))with two-dimensional layered structure has been reported as a promising catalyst for N_(2)fixation.Herein,to further enhance its NRR activity,a general doping strategy is developed to introduce and modulate the crystal defects of Bi_(2)Te_(3)nanosheets by adjusting the amount of Ce dopant(denoted as Ce_(x)-Bi_(2)Te_(3),where x represents the designed molar ratio of Ce/Bi).Meanwhile,the crystal defects can be designed and controlled by means of ion substitution and charge compensation.At−0.60 V versus the reversible hydrogen electrode(RHE),Ce_(0.3)-Bi_(2)Te_(3)exhibits a high NH_(3) yield(78.2μg·h^(−1)·mgcat^(−1)),a high FE(19.3%),excellent structural and electrochemical stability.Its outstanding catalytic activity is attributed to the tunable crystal defects by Ce doping.This work not only contributes to enhancing the NRR activity of Bi_(2)Te_(3)nanosheets,but also provides a reliable approach to prepare high-performance electrocatalysts by controlling the type and concentration of crystal defects for artificial N_(2)fixation.

关键词： electrochemical ammonia synthesis nitrogen reduction reaction (bismuth telluride)Bi_(2)Te_(3)nanosheets Ce doping crystal defects

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Engineering DNA logic systems with non-canonical DNA-nanostructures:basic principles,recent developments and bio-applications

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Science China Chemistry 2022年第2期65卷 284-297页

作者： Daoqing Fan Jun Wang Jiawen Han Erkang Wang shaojun dong State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Key Laboratory of Marine Drugs Ministry of EducationSchool of Medicine and PharmacyOcean University of China Laboratory for Marine Drugs and Bioproducts Pilot National Laboratory for Marine Science and TechnologyQ

Engineering DNA logic systems is considered as one of the most promising strategies for next-generation molecular computers.Owing to the inherent features of DNA,such as low cost,easy synthesis,and controllable hybridization,various DNA logic devices with different functions have been developed in the recent decade.Besides,a variety of logic-programmed biological applications are also explored,which initiates a new chapter for DNA logic computing.Although this field has gained rapid developments,a systematical review that could not only elaborate the logic principles of diverse DNA logic devices but also outline recent representative works is urgently needed.In this review,we first elaborate the general classification and logical principle of diverse DNA logic devices,in which the operating strategy of these devices and representative examples are selectively presented.Then,we review state-of-the-art advancements in DNA computing based on different non-canonical DNA-nanostructures during the past decade,in which some classical works are summarized.After that,the innovative applications of DNA computing to logic-controlled bioanalysis,cell imaging,and drug load/delivery are selectively presented.Finally,we analyze current obstacles and suggest appropriate prospects for this area.

关键词： DNA logic systems molecular logic non-canonical DNA-nanostructures arithmetic/non-arithmetic functions logical bio-applications

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Diatomic Fe-Fe catalyst enhances the ability to degrade organic contaminants by nonradical peroxymonosulfate activation system

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Nano Research 2023年第4期16卷 4678-4684页

作者： Minghua Li Jinxing Chen Weiwei Wu Shuangli Wu Lili Xu shaojun dong College of Chemistry Jilin UniversityChangchun 130012China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China

Atomically dispersed catalysts have been widely studied due to their high catalytic activity and atom utilization.Single-atom catalysts have achieved breakthrough progress in the degradation of emerging organic contaminants(EOCs)by activating peroxymonosulfate(PMS).However,the construction of atomically dispersed catalysts with diatomic/multiatomic metal active sites by activating PMS to degrade pollutants is still seldom reported,despite the unique merits of atom-pair in synergistic electronic modulation and breaking stubborn restriction of scaling relations on catalytic activity.We have synthesized Fe1-N-C,Fe_(2)-N-C,and Fe_(3)-N-C catalysts with monoatomic iron,diatomic iron,and triatomic iron active center,respectively.The results show that the catalytic degradation activity of Fe_(2)-N-C is twice that of Fe1-N-C and Fe_(3)-N-C due to its unique Fe_(2)N6 coordination structure,which fulfilled the complete degradation of rhodamine B(RhB),bisphenol A(BPA),and 2,4-dichlorophenol(2,4-DP)within 2 min.Electron paramagnetic resonance(EPR)and radical quenching experiments confirmed that the reaction was a nonradical reaction on the catalyst surface.And singlet oxygen and Fe(IV)are the key active species.

关键词： diatomic catalyst peroxymonosulfate nonradical contaminant

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A new FTO/TiO_(2)/PbO_(2)electrode for eco-friendly electrochemical determination of chemical oxygen demand

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Nano Research 2023年第8期16卷 11042-11047页

作者： Lei Wang Yuehan Zhang Xiaoxuan Sun Yunhui Li Junfeng Zhai shaojun dong School of Chemistry and Environmental Engineering Changchun University of Science and TechnologyChangchun 130022China Zhongshan Institute of Changchun University of Science and Technology Zhongshan 528437China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China College of Chemistry Jilin UniversityChangchun 130012China

Eco-friendly chemical oxygen demand(COD)sensors are highly desired with respect to the importance of COD determination in environmental protection.In this work,a new FTO/TiO_(2)/PbO_(2)(FTO=fluorine-doped tin oxide)electrode was fabricated with a two-step method and used as an eco-friendly electrochemical COD sensor.The interlayer TiO_(2)was employed to strengthen the adhesion of PbO_(2)on the FTO substrates by providing a large TiO_(2)/PbO_(2)interface area.The effects of the factors including applied potential,supporting electrolyte concentration and stirring speed on the sensing performance were investigated.Under the optimized conditions,linear responses to the COD of water with different COD sources were achieved,and a linear range from 5 to 120 mg/L was obtained in the case of sucrose as the COD source.The relative standard deviations(RSD)were determined to be less than 9%for the glucose solutions with the COD of 7.5,12.5 and 17.5 mg/L.For real sample analysis,the obtained results were comparable with those measured with the conventional dichromate method,with a relative error less than 11%.

关键词： chemical oxygen demand organic pollution chloride interference PbO_(2)electrode

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A revisiting of transition metal phosphide(Cu_(3)P and FeP)nanozymes for two sugar-related reactions

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Nano Research 2023年第1期16卷 189-194页

作者： Daiyong Chao Zhixuan Yu Jinxing Chen Qing dong Weiwei Wu Youxing Fang Ling Liu shaojun dong College of Chemistry Jilin UniversityChangchun 130012China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Transition metal phosphides(TMPs)are essential catalysts for some general catalytic reactions.However,their potentials for biological catalysis have seldom been explored.Herein,we investigated the enzyme-like properties of four TMPs(FeP,CoP,Ni_(2)P,and Cu_(3)P)towards two sugar-related reactions.Among the four TMPs,Cu_(3)P nanoparticles(NPs)efficiently catalyzed the hydrolysis of glycosidic bonds as glycoside hydrolase mimics,and FeP NPs possessed both glucose oxidase-like(GOx-like)and peroxidase-like activities,which combined into a cascade reaction for glucose’s simple and one-step colorimetric biosensor without GOx.Cu_(3)P and FeP NPs with distinctive enzyme-like activities have shown unique biological catalysis potentials for further applications with an attractive and challenging goal of developing nanomaterials to mimic natural enzymes,which encourages more efforts to reveal TMP’s capabilities towards biocatalysis.

关键词： transition metal phosphide glycoside hydrolase mimic glucose oxidase-like activity peroxidase-like activity cascade reaction

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Hierarchical porous nanosheets of Co-Mn bimetallic oxide from deep eutectic solvent for highly efficient peroxymonosulfate activation

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Nano Research 2023年第7期16卷 10381-10391页

作者： Jiale Wei Kai Rong Yuchen Wang Ling Liu Youxing Fang shaojun dong State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China

The development of highly active catalysts is the key to the successful application of sulfate radical(SO_(4)^(·-))-based advanced oxidation processes(AOPs)to wastewater treatment.Herein,bimetallic oxide CoMn_(2)O_(4)hierarchical porous nanosheets(CoMn_(2)O_(4)HPNSs)were constructed using glucose/urea deep eutectic solvent(DES)as sustainable solvent and self-formed sacrificial carbon templates.The prepared CoMn_(2)O_(4)HPNS exhibited outstanding peroxymonosulfate(PMS)activation performance,achieving the rapid degradation of refractory organic compounds in wastewater,including 5-sulfosalicylic acid(100%),acetaminophen(100%),oxtetracycline(100%),and sulfamethoxazole(91%)within 20 min.This excellent performance was attributed not only to the synergistic catalytic effect of Co-Mn bimetals,but also to the hierarchical porous structure which exposes more active sites and accelerates the migration of PMS and organic pollutants.In addition,CoMn_(2)O_(4)HPNS also showed excellent reusability and high stability in multiple cycles of degradation.The active species quenching results and electron paramagnetic resonance measurements revealed that SO_(4)^(·-)greatly contributed to organic degradation,while^(1)O_(2)and·OH also involved.Moreover,a series of other transition metal oxides(Co_(3)O_(4),Fe_(2)O_(3),Mn_(3)O_(4),NiO,and CoFe_(2)O_(4))with hierarchical porous nanosheet structures were successfully fabricated with this method.This study provides a simple,general,and low-cost strategy for fabricating hierarchical porous transition metal oxides,which are promising for the environmental remediation or many other applications in the future.

关键词： CoMn_(2)O_(4) hierarchical porous nanosheet 5-sulfosalicylic acid peroxymonosulfate deep eutectic solvent

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Atomically dispersed hierarchically ordered porous Fe-N-C single-atom nanozymes for dyes degradation

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Nano Research 2023年第8期16卷 10840-10847页

作者： Shuangli Wu Weiwei Wu Xinyang Zhu Minghua Li Jianguo Zhao shaojun dong Changchun State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China College of Chemistry Jilin UniversityChangchun 130012China

The development of novel nanozymes for environmental contamination remediation is a worthwhile research direction.However,most of the reported nanozymes cannot degrade efficiently due to the limitation of the internal active sites not being able to come into direct contact with contaminants.Therefore,we reported Fe-N-C single-atom nanozymes(SAzymes)with atomically dispersed FeN4 active sites anchored on a three-dimensional hierarchically ordered microporous-mesoporous-macroporous nitrogen doped carbon matrix(3DOM Fe-N-C)for the degradation of a targeted environmental pollutant(rhodamine B(RhB)).The three-dimensional(3D)hierarchically ordered porous structure may accelerate mass transfer and improve the accessibility of active sites.This structure and high metal atom utilization endow Fe-N-C SAzyme with enhanced tri-enzyme-mimic activities,comprising oxidase-mimic,peroxidase-mimic,and catalase-mimic activities.Based on its excellent peroxidase-mimic activity,3DOM Fe-N-C can degrade RhB by hydroxyl radicals(·OH)generated in the presence of hydrogen peroxide.This study provides a new idea for designing porous Fe-N-C SAzymes for environmental contamination remediation.

关键词： single-atom nanozymes(SAzymes) metal organic frameworks(MOFs) hierarchically ordered porous structure trienzyme mimics environmental contamination remediation

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High-performance liquid metal electromagnetic actuator fabricated by femtosecond laser

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International Journal of Extreme Manufacturing 2024年第2期6卷 511-521页

作者： Yiyu Chen Hao Wu Rui Li shaojun Jiang Shuneng Zhou Zehang Cui Yuan Tao Xinyuan Zheng Qianqian Zhang Jiawen Li Guoqiang Li dong Wu Jiaru Chu Yanlei Hu CAS Key Laboratory of Mechanical Behavior and Design of Materials Key Laboratory of Precision Scientific Instrumentation of Anhui Higher Education InstitutesDepartment of Precision Machinery and Precision InstrumentationUniversity of Science and Technology of ChinaHefei 230027People’s Republic of China Key Laboratory of Testing Technology for Manufacturing Process of Ministry of Education Southwest University of Science and TechnologyMianyang 621010People’s Republic of China Department of Mechanical Engineering The University of Hong KongHong Kong Special Administrative Region of ChinaPeople’s Republic of China

Small-scale electromagnetic soft actuators are characterized by a fast response and simplecontrol,holding prospects in the field of soft and miniaturized robotics.The use of liquid metal(LM)to replace a rigid conductor inside soft actuators can reduce the rigidity and enhance the actuation performance and robustness.Despite research efforts,challenges persist in the flexible fabrication of LM soft actuators and in the improvement of actuation performance.To address these challenges,we developed a fast and robust electromagnetic soft microplate actuator based on a laser-induced selective adhesion transfer method.Equipped with unprecedentedly thin LM circuit and customized low Young’s modulus silicone rubber(1.03 kPa),our actuator exhibits an excellent deformation angle(265.25?)and actuation bending angular velocity(284.66 rad·s^(-1)).Furthermore,multiple actuators have been combined to build an artificial gripper with a wide range of functionalities.Our actuator presents new possibilities for designing small-scaleartificial machines and supports advancements in ultrafast soft and miniaturized robotics.

关键词： soft actuators femtosecond laser liquid metal

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Deep eutectic solvent assisted facile synthesis of low-dimensional hierarchical porous high-entropy oxides

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Nano Research 2022年第3期15卷 2756-2763页

作者： Jiale Wei Kai Rong Xiaolong Li Yuchen Wang Zhen-An Qiao Youxing Fang shaojun dong State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry International Joint Research Laboratory of Nano-Micro Architecture ChemistryCollege of ChemistryJilin University2699 Qianjin StreetChangchun 130012China

High-entropy-oxides(HEOs),a new class of solids that contain five or more elemental species,have attracted increasing interests owing to their unique structures and fascinating physicochemical properties.However,it is a huge challenge to construct various nanostructured,especially low-dimensional nanostructured HEOs under the high temperature synthetic conditions.Herein,a facile strategy using glucose-urea deep eutectic solvent(DES)as both a solvent and the carbon source of structure-directed template is proposed for the synthesis of various HEOs with two-dimentional(2D)nanonets and one-dimentional(1D)nanowires,including rock-salt(Co,Cu,Mg,Ni,Zn)O,spinel(Co,Cr,Fe,Mn,Ni)_(3)O_(4),and perovskite La(Co,Cr,Fe,Mn,Ni)O_(3).The as-prepared HEOs possessed five or more uniformly dispersed metal elements,large specific surface areas(more than 25 m^(2)·g^(−1)),and a pure single-phase structure.In addition,high cooling rate(cooling in air or liq-N_(2)-quenching)was indispensable to obtain a single-phase rock-salt(Co,Cu,Mg,Ni,Zn)O because of phase separation caused by copper.By taking advantage of unique features of HEOs,rock-salt(Co,Cu,Mg,Ni,Zn)O can function as a promising candidate for lithium-ion batteries(LIBs)anode material,which achieved excellent cycling stability.This work provides a feasible synthetic strategy for low-dimensional hierarchical HEOs,which creates new opportunities for the stable HEOs being highly active functional materials.

关键词： high-entropy oxide deep eutectic solvent one-/two-dimentional(1D/2D)hierarchical structure lithium-ion battery

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One-step synthesis of three-dimensional mesoporous Co_(3)O_(4)@Al_(2)O_(3)nanocomposites with deep eutectic solvent:An efficient and stable peroxymonosulfate activator for organic pollutant degradations

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Nano Research 2023年第8期16卷 11430-11443页

作者： Yuchen Wang Kai Rong Jiale Wei Shanlei Chang Dengbin Yu Youxing Fang shaojun dong State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China College of Chemistry Jilin UniversityChangchun 130022China

The effective,stable,and secure catalysts are essential for sulfate radical(SO_(4)·−)-based advanced oxidation processes(SR-AOPs)to the degradation of organic contaminants in water.Heterogeneous supported cobalt-based catalysts are commonly used to activate peroxymonosulfate(PMS)to achieve the degradation.In this work,we synthesized Co_(3)O_(4)@Al_(2)O_(3)three-dimensional(3D)mesoporous nanocomposite(denoted as Co_(3)O_(4)@Al_(2)O_(33)DPNC)in just one step by calcining cheap and green deep eutectic solvent(DES)solution containing Co salt.Co_(3)O_(4)@Al_(2)O_(33)DPNC with the high specific surface area(93.246 m^(2)/g),uniform pore distribution(3.829 nm)and rich porosity(0.255 cm^(3)/g)were attained in a beautiful hierarchical structure which exhibited the open 3D propeller-like microstructure,two-dimensional lamellar substructure with rich folds,as well as the decoration of highly dispersed Co_(3)O_(4)nanoparticles on mesoporous amorphous Al_(2)O_(3).The excellent chemical and thermal stability of Al_(2)O_(3)ensures the high stability of the catalyst,and the formation of the complex hierarchical structure makes the active Co_(3)O_(4)be homogenously dispersed for effective catalysis.The catalyst demonstrated outstanding performance for catalytic degradations of organic pollutants(acetaminophen,oxytetracycline,5-sulfosalicylic acid,orange G and Rhodamine B)by generated SO_(4)·−,·OH and^(1)O_(2).With a very low cobalt content(equal to 28.2 mg/L of Co),the catalyst exhibited very high stability and excellent reusability in the recycling usages,while the leaching of the cobalt element(<0.145 mg/L)was also at a low level.Our catalyst achieved effective degradations of acetaminophen in cycles without losing its stable hierarchical nanostructure.

关键词： peroxymonosulfate organic pollutant degradation deep eutectic solvent Co_(3)O_(4)@Al_(2)O_(3)nanocomposite hierarchical nanostructure

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