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Photocatalytic and Electrocatalytic Generation of Hydrogen Peroxide: Principles, Catalyst Design and Performance

Nano-Micro Letters 2023年第6期15卷 24-72页

作者： Yan Guo Xili Tong Nianjun yang State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001People’s Republic of China University of Chinese Academy of Sciences Beijing 100049People’s Republic of China Institute of Materials Engineering University of Siegen57076 SiegenGermany Department of Chemistry Hasselt University3590 DiepenbeekBelgium IMO‑IMOMEC Hasselt University3590 DiepenbeekBelgium

Hydrogen peroxide(H_(2)O_(2)) is a high-demand organic chemical reagent and has been widely used in various modern industrial applications. Currently,the prominent method for the preparation of H_(2)O_(2) is the anthraquinone oxidation.Unfortunately, it is not conducive to economic and sustainable development since it is a complex process and involves unfriendly environment and potential hazards. In this context, numerous approaches have been developed to synthesize H_(2)O_(2). Among them, photo/electro-catalytic ones are considered as two of the most promising manners for on-site synthesis of H_(2)O_(2). These alternatives are sustainable in that only water or O_(2) is required. Namely, water oxidation(WOR) or oxygen reduction(ORR)reactions can be further coupled with clean and sustainable energy. For photo/electro-catalytic reactions for H_(2)O_(2) generation, the design of the catalysts is extremely important and has been extensively conducted with an aim to obtain ultimate catalytic performance. This article overviews the basic principles of WOR and ORR,followed by the summary of recent progresses and achievements on the design and performance of various photo/electro-catalysts for H_(2)O_(2) generation. The related mechanisms for these approaches are highlighted from theoretical and experimental aspects. Scientific challenges and opportunities of engineering photo/electro-catalysts for H_(2)O_(2) generation are also outlined and discussed.

关键词： H_(2)O_(2)generation Photocatalysts Electrocatalysts Reaction mechanisms

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Tailoring interfacial electron redistribution of Ni/Fe_(3)O_(4) electrocatalysts for superior overall water splitting

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Journal of Energy Chemistry 2022年第10期31卷 330-338,I0008页

作者： Wenli Xu Wenda Zhong Chenfan yang Rong Zhao Jing Wu Xuanke Li Nianjun yang Hubei Province Key Laboratory of Coal Conversion and New Carbon Materials Wuhan University of Science and TechnologyWuhan 430081HubeiChina Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology Hunan UniversityChangsha 410082HunanChina Institute of Materials Engineering University of SiegenSiegen 57076Germany

Exploring highly active earth-abundant bifu nctional electrocatalysts for water splitting at a high output is essential for the forthcoming hydrogen economy.Non-noble Fe_(3)O_(4) catalyst owns outstanding conductivity and its octahedral Fe sites can markedly promote water dissociation.However,it lacks active centers on the surface,resulting in its poor activity when used as a catalyst for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Herein,an electron redistribution strategy is proposed by introducing Ni sites onto the surface of Fe_(3)O_(4)(Ni/Fe_(3)O_(4)).The abundant delocalized electrons,derived from the electronic interaction of Ni and Fe_(3)O_(4) species,significantly optimize the electronic structure of the Ni/Fe_(3)O_(4) catalyst,leading to its improved adsorption behavior.This Ni/Fe_(3)O_(4) catalyst exhibits remarkable bifunctional activity,steadily outputting 1000 mA cm^(-2)at the low overpotential of 387 mV for HER and 338 mV for OER,respectively.Using Ni/Fe_(3)O_(4) as a bifunctional catalyst for overall water splitting reaction exhibits the optimal performance with outstanding stability,obtaining a current density of1000 mA cm^(-2)at 1.98 V,much superior to a Pt/C‖IrO_(2)cell.Experimental analysis and theoretical calculations collectively corroborate that the electron redistribution of Fe_(3)O_(4) is activated by coupling Ni species,leading to the promoted HER and OER kinetics.This electron redistribution strategy provides an effective method to activate transition metal-based catalysts which are promising to be utilized as superior electrocatalysts for the industrial overall water splitting reaction.

关键词： Electron redistribution Ni/Fe_(3)O_(4)heterojunction Overall water splitting

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High C–C cleavage efficiencies of ethanol oxidation reaction on mesoporous RhPt electrocatalysts

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SusMat 2022年第6期2卷 689-698页

作者： Sufang yang Xiaobo yang Xueqin Cui Xinhua Gao Houbing Zou Xili Tong Nianjun yang State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuanChina University of Chinese Academy of Sciences BeijingChina School of Chemistry and Chemical Engineering Shanxi UniversityTaiyuanChina NingXia University YinchuanChina Institute of Materials Engineering University of SiegenSiegenGermany

Optimizing the structure of an electrocatalyst is critical to achieve its outstand-ing performance as well as to establish relationships between its composition and its performance.In this work,a series of mesoporous RhPt electrocatalysts(RhPt-MPS)with different compositions are designed and synthesized toward the ethanol oxidation reaction(EOR).The mesoporous structure of RhPt-MPS exposes abundant surface sites and channels for mass transfer of ethanol,and thus boosts the catalytic EOR performance.It has been confirmed that Rh not only reduces the oxidation potential of EOR,but also effectively facilitates the breakage of C-C bond.Stemming from structural and compositional advantages of the RhPt 0.6-MPS electrocatalyst,it exhibits the highest activity(2846.0 mA mg^(–1))for the EOR when compared with other RhPt-MPS,Rh-MPS,and Pt-MPS electrocatalysts.It also delivers excellent stability and high selectivity than other electrocatalysts.

关键词： C-Cbondsplitting electrocatalysts ethanolelectro-oxidationreaction mesoporousmaterials RhPt

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On-Chip Micro Temperature Controllers Based on Freestanding Thermoelectric Nano Films for Low-Power Electronics

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Nano-Micro Letters 2024年第7期16卷 98-108页

作者： Qun Jin Tianxiao Guo Nicolas Perez Nianjun yang Xin Jiang Kornelius Nielsch Heiko Reith Institute for Metallic Materials Leibniz Institute for Solid State and Materials Research01069 DresdenGermany Institute of Materials Engineering University of Siegen57076 SiegenGermany Institute of Applied Physics Technical University of Dresden01069 DresdenGermany Institute of Materials Science Technical University of Dresden01069 DresdenGermany

Multidimensional integration and multifunctional com-ponent assembly have been greatly explored in recent years to extend Moore’s Law of modern microelectronics.However,this inevitably exac-erbates the inhomogeneity of temperature distribution in microsystems,making precise temperature control for electronic components extremely challenging.Herein,we report an on-chip micro temperature controller including a pair of thermoelectric legs with a total area of 50×50μm^(2),which are fabricated from dense and flat freestanding Bi2Te3-based ther-moelectric nano films deposited on a newly developed nano graphene oxide membrane substrate.Its tunable equivalent thermal resistance is controlled by electrical currents to achieve energy-efficient temperature control for low-power electronics.A large cooling temperature difference of 44.5 K at 380 K is achieved with a power consumption of only 445μW,resulting in an ultrahigh temperature control capability over 100 K mW^(-1).Moreover,an ultra-fast cooling rate exceeding 2000 K s^(-1) and excellent reliability of up to 1 million cycles are observed.Our proposed on-chip temperature controller is expected to enable further miniaturization and multifunctional integration on a single chip for microelectronics.

关键词： Temperature control Low-power electronics On-chip micro temperature controller Freestanding thermoelectric nano films Temperature-sensitive components

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Construction of high stability indium gallium zinc oxide transistor biosensors for reliable detection of bladder cancer-associated microRNA

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Chinese Chemical Letters 2022年第2期33卷 979-982页

作者： Jing Guo Ruichen Shen Xuejie Shen Bo Zeng Nianjun yang Huageng Liang Yanbing yang Quan Yuan Key Laboratory of Biomedical Polymers of Ministry of Education College of Chemistry and Molecular SciencesSchool of MicroelectronicsWuhan UniversityWuhan 430072China Department of Urology Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430022China Institute of Chemical Biology and Nanomedicine State Key Laboratory of Chemo/Biosensing and ChemometricsCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China Institute of Materials Engineering University of SiegenSiegen 57076Germany

Bladder cancer is the most common malignant tumours with high morbidity, mortality and recurrence.However, currently developed detection methods for bladder cancer-associated urine biomarkers are hindered by their extremely low abundance. Hence, the exploration of a highly sensitive and selective approach for the detection of trace bladder cancer-associated biomarkers in human urine is of vital importance for the diagnosis of bladder cancer. Herein, we developed a highly reliable indium gallium zinc oxide field effect transistor(IGZO FET) biosensor for the detection of bladder cancer-related biomarker micro RNA. The single-stranded DNA-functionalized IGZO FET biosensors exhibit high sensing reproducibility and stability with an ultralow detection limit of 19.8 amol/L. The device could also be used for quantitative detection of trace micro RNA in human urine samples and can effectively distinguish bladder cancer patients from healthy donors. The development of high performance IGZO FET biosensors presents new opportunities for the achievement of early-stage diagnosis of bladder cancer.

关键词： Bladder cancer Field-effect transistors IGZO miRNA Urine

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Cobalt-iron oxide/black phosphorus nanosheet heterostructure:Electrosynthesis and performance of(photo-)electrocatalytic oxygen evolution

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Nano Research 2023年第5期16卷 6057-6066页

作者： Man Zhao Xiaoru Cheng He Xiao Jianru Gao Shoufeng Xue Xiaoxia Wang Haishun Wu Jianfeng Jia Nianjun yang Key Laboratory of Magnetic Molecules&Magnetic Information Materials Ministry of Education The School of Chemical and Material ScienceShanxi Normal UniversityTaiyuan 030000China Institute of Materials Engineering University of SiegenSiegen 57076Germany

Highly active,stable,and cut-price(photo-)electrocatalysts are desired to overwhelm high energy barriers for anodic oxygen evolution reaction processes.Herein,a heterostructure of cobalt-iron oxide/black phosphorus nanosheets is in-situ synthesized via a facile and novel three-electrode electrolysis method.Bulky black phosphorus is exfoliated into its nanosheets at the cathode while the CoFe oxide is derived directly from the metal wire anode during the electrolysis process.This heterostructure exhibits excellent electrocatalytic oxygen evolution reaction(OER)performance,and the overpotential at 10 mA·cm^(−2)is 51 mV lower than that of the commercial RuO_(2)catalyst.Its superior OER performance stems from the favorable adsorption behavior and an enlarged electrochemical active surface area of the catalyst.To reveal the origin of excellent OER performance from the point of adsorption strength of OH*,methanol oxidation reaction(MOR)test is applied under the identified OER operating conditions.Further introduction of light illumination enhances the OER activity of this heterostructure.The overpotential drops down to 280 mV,benefiting from pronounced photochemical response of black phosphorus nanosheets and iron oxide inside the heterostructure.This work develops a new electrochemical method to construct high performance and light-sensitive heterostructures from black phosphorus nanosheets for the OER.

关键词： electrosynthesis oxygen evolution reaction black phosphorus cobalt oxide iron oxide

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Tailoring synergetic catalytic interface of VPO/Ni_(2)P to boost hydrogen evolution under alkaline conditions

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Journal of Energy Chemistry 2022年第2期31卷 674-680页

作者： Wenli Xu Qiqi Li Wenda Zhong Bing Sun Qiang Huang Xu Nan Yinhong Gao Yao yang Qin Zhang Nianjun yang Xuanke Li School of Chemistry and Chemical Engineering Wuhan University of Science and TechnologyWuhan 430081HubeiChina Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology Hunan UniversityChangsha 410082HunanChina Institute of Materials Engineering University of SiegenSiegen 57076Germany

Design of the catalyst for efficient water dissociation and hydrogen recombination is paramount in enhancement of the alkaline water electrolysis kinetics.Herein,we reported a delicate hierarchical(VO)_(2) P_(2)O_(7)-Ni_(2) P@NF(VPO-Ni_(2) P@NF)hybrid catalyst that operated efficiently in alkaline media.The VPO and Ni_(2) P respectively act as the water dissociation promoter and the hydrogen recombination center,which synergistically propel water adsorption/dissociation and H intermediates recombination.The resulting synergistic interfaces between VPO and Ni_(2) P are verified to afford the catalyst an outstanding performance for hydrogen evolution reaction in alkaline media with an overpotential of 154 mV at 10 mA cm^(-2),Tafel slope of 65 mV dec^(-1),and remarkable durability.Furthermore,the catalyst presents the potential for overall water splitting.This work may shed fresh light on the high-performance electrocatalyst design and the application of VPO on water electrolysis.

关键词： Alkaline water electrolysis Interface engineering (VO)_(2)P_(2)O_(7) Ni_(2)P

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Revealing component synergy of Ni‒Fe/black phosphorous composites synthesized by self-designed electrochemical method for enhancing photoelectrocatalytic oxygen evolution reaction

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Frontiers of Materials Science 2023年第2期17卷 143-153页

作者： He Xiao Shoufeng Xue Zimei Fu Man Zhao Li Zhang Junming Zhang Haishun Wu Jianfeng Jia Nianjun yang Key Laboratory of Magnetic Molecules&Magnetic Information Materials(Ministry of Education) School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032China Department of Chemistry Hasselt University3590 DiepenbeekBelgium

Developing high-activity and low-cost catalysts is the key to eliminate the limitation of sluggish anodic oxygen evolution reaction(OER)during electrocatalytic overall water splitting.Herein,Ni‒Fe/black phosphorous(BP)composites are synthesized using a simple three-electrode system,where exfoliation of bulky BP and synthesis of NiFe composites are simultaneously achieved.Under light illumination,the optimized Ni‒Fe/BP composite exhibits excellent photoelectrocatalytic OER performance(e.g.,the overpotential is 58 mV lower than a commercial RuO_(2) electrocatalyst at a current density of 10 mA·cm^(-2)).The electron transfer on this composite is proved to follow a Ni‒BP‒Fe pathway.The electronic structure of this Ni‒Fe/BP composite is effectively regulated,leading to optimized adsorption strength of the intermediate OH*and improved intrinsic activity for the OER.Together with active sites on the support,this Ni‒Fe/BP composite possesses abundant electrochemical active sites and a bug surface area for the OER.The introduction of light further accelerates the electrocatalytic OER.This work provides a novel and facile method to synthesize high-performance metal/BP composites as well as the approaches to reveal their OER mechanisms.

关键词： black phosphorous (photo-)electrocatalysis oxygen evolution reaction

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Polyanionic hydrogel electrolyte enables reversible and durable Zn anode for efficient Zn-based energy storage

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Journal of Energy Chemistry 2023年第11期86卷 373-381,I0008页

作者： Chunjiang Jin Congcong yang Hongyu Mi Chenchen Ji Fengjiao Guo Chengzhe Liu Ziqiang Liu Nianjun yang State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources School of Chemical Engineering and TechnologyXinjiang UniversityUrumqi 830017XinjiangChina Department of Chemistry Hasselt UniversityDiepenbeek 3590Belgium

Aqueous Zn-ion energy storage systems,which are expected to be integrated into intelligent electronics as a secure power supply,suffer poor reversibility of Zn anodes,predominantly associated with dendritic growth and side reactions.This study introduces a polyanionic strategy to address these formidable issues by developing a hydrogel electrolyte(PACXHE)with carboxyl groups.Notably,the carboxyl groups within the hydrogel structure establish favorable channels to promote the transport of Zn^(2+)ions.They also expedite the desolvation of hydrated Zn^(2+)ions,leading to enhanced deposition kinetics.Additionally,these functional groups confine interfacial planar diffusion and promote preferential deposition along the(002)plane of Zn,enabling a smooth surface texture of the Zn anode.This multifaceted regulation successfully achieves the suppression of Zn dendrites and side reactions,thereby enhancing the electrochemical reversibility and service life during plating/stripping cycles.Therefore,such an electrolyte demonstrates a high average Coulombic efficiency of 97.7%for 500 cycles in the Zn‖Cu cell and exceptional cyclability with a duration of 480 h at 1 mA cm^(-2)/1 mA h cm^(-2)in the Zn‖Zn cell.Beyond that,the Zn-ion hybrid micro-capacitor employing PACXHE exhibits satisfactory cycling stability,energy density,and practicality for energy storage in flexible,intelligent electronics.The present polyanionic-based hydrogel strategy and the development of PACXHE represent significant advancements in the design of hydrogel electrolytes,paving the way for a more sustainable and efficient future in the energy storage field.

关键词： Polyanionic hydrogel electrolyte Zinc anode issues Dendrite suppression Electrochemical performance Zinc-ionhybrid micro-capacitor

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Direct Electrochemistry of Hemoglobin on Vertically Aligned Carbon Hybrid TiO2 Nanotubes and Its Highly Sensitive Biosensor Performance

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Chinese Journal of Chemistry 2013年第2期31卷 215-220页

作者： Meichuan Liu Guohua Zhao Yiting Tang Huijie Shi Nianjun yang Department of Chemistry Tongji University Shanghai 200092 China Key Laboratory of yangtze River Water Environment Ministry of Education Tongji University Shanghai 200092 China 1m2

The present work is focused on developing a novel biomaterial platform to achieve enhanced direct electron transfer （DET） of hemoprotein and higher biosensor performance on vertically aligned carbon hybrid TiO2 nanotubes （C-TiO2 NTs）. Using a simple surfactant-assisted method, controllable hybridization of TiO2 NTs with conductive amorphous carbon species is realized. The obtained C-TiO2 NTs is ingeniously chosen to serve as an ideal ＂vessel＂ for protein immobilization and biosensor applications. Results show that the appropriate hybridization of C into TiO2 NTs leads to a much better conductivity of TiO2 NTs without destroying their preponderant tubular structures or damaging their excellent biocompatibility and hydrophilicity. When used in loading proteins, the C-TiO2 NTs can be used as a super vessel for rapid and substantive immobilization of hemoglobin （Hb）, with a large surface electroactive Hb coverage （I＊） of 3.3 × 10 9 mol·cm^-2. Enhanced DET of Hb is commendably observed on the constructed Hb/C-TiO2 NTs biosensor with a couple of well-defined redox peaks in a fast electron transfer process. The biosensor further exhibits fast response, high sensitivity and stability for the amperometric biosensing of H202 with the detection limit as low as 3.1 × 10^-8 mol/L.

关键词： carbon hybrid TiO2 nanotubes direct electron transfer electrochemical biosensors hemoglobin

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