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Interfacial engineering of SnO_(2)/Bi_(2)O_(2)CO_(3)heterojunction on heteroatoms-doped carbon for high-performance CO_(2)electroreduction to formate

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Nano Research 2023年第2期16卷 2278-2285页

作者： Danni Wang Tingting Sun Lianbin Xu Lei Gong Baotong Chen Pianpian Zhang Tianyu Zheng Qingmei Xu Houhe Pan Yuexing Zhang Jianzhuang Jiang Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China College of Chemistry and Chemical Engineering Dezhou UniversityDezhou 253023China

Electrochemical CO_(2)reduction is a viable,economical,and sustainable method to transform atmospheric CO_(2)into carbon-based fuels and effectively reduce climate change and the energy crisis.Constructing robust catalysts through interface engineering is significant for electrocatalytic CO_(2)reduction(ECR)but remains a grand challenge.Herein,SnO2/Bi_(2)O_(2)CO_(3)heterojunction on N,S-codoped-carbon(SnO_(2)/BOC@NSC)with efficient ECR performance was firstly constructed by a facile synthetic strategy.When the SnO_(2)/BOC@NSC was utilized in ECR,it exhibits a large formic acid(HCOOH)partial current density(JHCOOH)of 86.7 mA·cm^(−2)at−1.2 V versus reversible hydrogen electrode(RHE)and maximum Faradaic efficiency(FE)of HCOOH(90.75%at−1.2 V versus RHE),respectively.Notably,the FEHCOOH of SnO_(2)/BOC@NSC is higher than 90%in the flow cell and the JHCOOH of SnO_(2)/BOC@NSC can achieve 200 mA·cm^(−2)at−0.8 V versus RHE to meet the requirements of industrialization level.The comparative experimental analysis and in-situ X-ray absorption fine structure reveal that the excellent ECR performance can be ascribed to the synergistic effect of SnO_(2)/BOC heterojunction,which enhances the activation of CO_(2)molecules and improves electron transfer.This work provides an efficient SnO_(2)-based heterojunction catalyst for effective formate production and offers a novel approach for the construction of new types of metal oxide heterostructures for other catalytic applications.

关键词： heterojunction charge transfer electrochemical CO_(2)reduction flow cell in-situ X-ray absorption fine structure

Tensile stress enhanced dynamic oxygen vacancies on interlayer stretched Bi_(2)O_(2)CO_(3) as pivotal knobs to promote sustainable selective CO_(2) photoreduction

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能源化学:英文版 2023年第8期83卷 173-179,I0006页

作者： Xian Shi Weidong Dai Xing'an Dong Qin Ren Ping Yan Fan Dong School of Chemistry and Environmental Engineering Sichuan University of Science&EngineeringZigong 643000SichuanChina Research Center for Carbon-Neutral Environmental&Energy Technology Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 611731SichuanChina State Centre for International Cooperation on Designer Low-Carbon and Environmental Materials(CDLCEM) School of Materials Science and EngineeringZhengzhou UniversityZhengzhou450001HenanChina College of Architecture and Environment Sichuan UniversityChengdu 610065SichuanChina

Surface oxygen vacancies(OVs) with abundant localized electrons on bismuth-oxygen based photocatalysts are proved to have the ability to capture and activate CO_(2).However,the surface OVs are easily filled with oxygen-containing species and destroyed,losing their effects as active sites and hindering the subsequent CO_(2)photoreduction.For realistic and sustainable CO_(2)photoreduction,constructing sustainable and stable surface OVs as active sites on photocatalysts is essential.This work shows the synthesis of interlayer stretched Bi_(2)O_(2)CO_(3) ultrathin nanosheets with tensile stress,which are beneficial to continuously generating light-induced dynamic OVs.With sufficient active sites,excellent,stable,and selective photoreduction of CO_(2)to CO under simulated solar light is achieved.The light-induced OVs can reduce the energy barrier of rate-determining step,resulting in the 100% product selectivity.The results presented herein demonstrate the effect of dynamic OVs induced by interlayer tensile strain on catalysts for the enhanced selective CO_(2)photoreduction process.

关键词： Ultrathin Bi_(2)O_(2)CO_(3) Dynamic oxygen vacancies Product selectivity charge transfer CO_(2) phororeduction

SERS and EC dual-mode detection for dopamine based on WO_(3)-SnO_(2)nanoflake arrays

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Nano Research 2023年第3期16卷 4049-4054页

作者： Linya Lu Yan Zhou Tingting Zheng Yang Tian School of Chemistry and Molecular Engineering East China Normal UniversityShanghai 200241China State Key Laboratory of Precision Spectroscopy East China Normal UniversityShanghai 200241China

As an important neurotransmitter,the detection of dopamine(DA)is of great significance for the diagnosis and treatment of neurological diseases.In this study,WO_(3)-SnO_(2)nanoflake arrays were synthesized on fluorine-doped tin oxide(FTO)by hydrothermal synthesis and pulse electrodeposition,revealing significant surface-enhanced Raman scattering(SERS)activity with an enhancement factor(EF)reaching 4.79×10^(7).The obvious EF was mainly ascribed to the charge transfer between WO_(3)-SnO_(2)and methylene blue(MB)based on chemical mechanism(CM)and the molecular resonance effect.With the competitive adsorption of DA and absorbed MB,we prepared a SERS and electrochemical(EC)dual-mode detection platform of DA based on the WO_(3)-SnO_(2)nanoflake arrays.The linear range(LR)was 5.00-1.75×10^(3)nmol/L,and the detection limits(LODs)were as low as 1.50 and 0.80 nmol/L by SERS and EC respectively.Besides,the developed detection platform can shield the interference of many neurotransmitters similar to DA,showing good selectivity and excellent stability.In general,the SERS-EC dual-mode detection platform can be well applied to the detection of DA in cell lysate,demonstrating great potential in diagnosis of neurodegenerative diseases.

关键词： surface enhanced Raman scattering electrochemical WO3-SnO2 nanoflake arrays charge transfer dopamine

Advanced heterolytic H_(2) adsorption of K-added Ru/MgO catalysts for accelerating hydrogen storage into aromatic benzyltoluenes

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Journal of Energy Chemistry 2022年第8期31卷 333-343,I0009页

作者： Tae Wan Kim Hwiram Jeong Yeongin Jo Dongun Kim Ji Hoon Park Seok Ki Kim Young-Woong Suh Department of Chemical Engineering Hanyang UniversitySeoul 04763Republic of Korea Environmental&Sustainable Resources Research Center Korea Research Institute of Chemical TechnologyDaejeon 34114Republic of Korea Department of Chemical Engineering Ajou UniversitySuwon 16499Republic of Korea

Herein,we report a highly active K-added Ru/MgO catalyst for hydrogen storage into aromatic benzyltoluenes at low temperatures to advance liquid organic hydrogen carrier technology.The hydrogenation activity of Ru/K/MgO catalysts exhibits a volcano-shaped dependence on the K content at the maximum with 0.02 wt%.This is in good agreement with the strength and capacity of H_(2) adsorption derived from basicity,despite a gradual decrease in the textural property and the corresponding increase in the Ru particle size with increasing the K content.Density functional theory calculations show that heterolytic hydrogen adsorption properties(strength and polarization)are facilitated up to a specific density of K on the Ru–MgO interface and excessive K suppresses heterolytic H_(2) adsorption by direct interaction between K and hydrogen,assuring the hydrogenation activity and H_(2) adsorption capability of Ru/K/MgO catalysts.Hence,the Ru/K/MgO catalyst,when K is added in an optimal amount,is highly effective to accelerate hydrogen storage kinetics at low temperatures owing to the enhanced heterolytic H_(2) adsorption.

关键词： Chemical hydrogen storage Supported Ru catalysts Ru–MgO interface Heterolytic H_(2)adsorption charge transfer Potassium promotion

charge-transfer Supra-amphiphiles Built by Water-Soluble Tetrathiafulvalenes and Viologen-Containing Amphiphiles

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Charge-Transfer Supra-amphiphiles Built by Water-Soluble Tet...

Constructing heterojunction interface of Co_(3)O_(4)/TiO_(2) for efficiently accelerating acetaminophen degradation via photocatalytic activation of sulfite

中国化学会第九届全国无机化学学术会议

作者： Zhongpeng Lv Bin Chen Haiying Wang Yue Wu Jinglin Zuo Department of Chemistry Nanjing University

Organogels or organic self-assemble nanostructures based on π-systems that have inherent electronic properties such as luminescence, charge carrier mobility, and electronic conductivity are extensively used for designing organic electronic devices such as LEDs, FETs and PVDs. Among these, organic low molecular weight gelators（LMWGs） with the famous sulfur-rich organic donor molecules, such as a tetrathiafulvalene derivatives（TTFs）, have received considerable attention because the formed gels usually exhibit redox active response and conducting or semiconducting properties. In this study, multidimensional nanoassemblies with various morphologies such as nanosheets, nanorods and nanofibers are developed via charge-transfer interaction and supra-amphiphile self-assembling in aqueous phase. The charge-transfer interactions between tetrathiafulvalene derivatives（TTFs） and methyl viologen derivatives（MVs） have been confirmed by the characteristic charger-transfer absorption. 1H NMR and ESI analyses also indicate supra-amphiphiles are formed by combination of TTFs and MVs head group through charge-transfer interaction and coulombian force. X-ray single crystal structural studies, HRTEM and SEM reveal that both linkage pattern of TTFs in hydrophilic part and alkane chain structure in hydrophobic part have significant influence on nanoassemblies morphology and microstructure. Moreover, gold nanoparticles（Au NPs） are introduced in the above supramolecular nanoassemblies to construct a supra-amphiphile driven organic-Au NPs assembly system. Au NPs could be assembled into 1-D to 3-D structures by adding different amount of MVs.

关键词： charge transfer supra-amphiphiles nanoassemblies multidimensional materials hybrid materials

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Chinese Chemical Letters 2023年第3期34卷 200-205页

作者： Qiangwei Li Mengmeng Zhang Yongyi Xu Xiaoqi Quan Yiao Xu Wen Liu Lidong Wang Department of Environmental Science and Engineering Hebei Key Lab of Power Plant Flue Gas Multi–Pollutants ControlNorth China Electric Power UniversityBaoding 071003China The Key Laboratory of Water and Sediment Sciences Ministry of EducationCollege of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China China Power Hua Chuang Electricity Technology Research Company Ltd. Suzhou 215123China

Achieving efficient degradation of organic pollutants via activation of sulfite is meaningful but challenging.Herein,we have constructed a heterogeneous catalyst system involving Co_(3)O_(4) and TiO_(2) nanoparticles to form the p-n heterojunction(Co_(3)O_(4)/TiO_(2)) to degrade acetaminophen(ACE) through photocatalytic activation of sulfite.Specifically,X-ray photoelectron spectroscopy analysis and theoretical calculations provide compelling evidence of electron transfer from Co_(3)O_(4) to TiO_(2) at the heterointerface.The interfacial electron redistribution of Co_(3)O_(4)/TiO_(2) tunes the adsorption energy of HSO_(3)^(-)/SO_(3)^(2-) in sulfite activation process for enhanced the catalytic activity.Owing to its unique heterointerface,the degradation efficiency of ACE reached 96.78%within 10 min.The predominant active radicals were identified as ·OH,h^(+),and SO_(x)^(·-) through radical quenching experiments and electron spin resonance capture.Besides,the possible degradation pathway was deduced by monitoring the generated intermediate products.Thereafter,the enhanced roles of well-engineered compositing interface in photocatalytic activation of sulfite for complete degradation of ACE were unveiled that it can improve light absorption ability,facilitate the generation of active species,and optimize reactive pathways.Considering that sulfite is a waste from flue gas desulfurization process,the photocatalytic activation of sulfite system will open up new avenues of beneficial use of air pollutants for the removal of pharmaceutical wastewater.

关键词： Sulfite Photocatalytic activation charge transfer Heterojunction interface Degradation mechanism

Sequential Growth of Cs_(3)Bi_(2)I_(9)/BiVO_(4)Direct Z-Scheme Heterojunction for Visible-Light-Driven Photocatalytic CO_(2)Reduction

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Transactions of Tianjin University 2023年第6期29卷 462-472页

作者： Long Jiang Hanrui Du Le Li Xiangjiu Guan Yihao Zhang Liwei Li Xiaoxu Liu Lei Li Yingcheng Tian Li Zhang Shuai Wang Jie Chen Shaohua Shen State Key Laboratory for Performance and Structure Safety of Petroleum Tubular Goods and Equipment Materials CNPC Tubular Goods Research InstituteXi’an 710077China International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an 710049China School of Chemical Engineering and Technology Xi’an Jiaotong UniversityXi’an 710049China CNPC National Engineering Research Center for Oil and Gas Drilling Equipment Co. Ltd.Baoji 721002China China Coal Energy Research Institute Co. Ltd.Xi’an 710049China

The high exciton binding energy and lack of a positive oxidation band potential restrict the photocatalytic CO_(2)reduction efficiency of lead-free Bi-based halide perovskites Cs_(3)Bi_(2)X_(9)(X=Br,I).In this study,a sequential growth method is presented to prepare a visible-light-driven(λ>420 nm)Z-scheme heterojunction photocatalyst composed of BiVO_(4)nanocrystals decorated on a Cs_(3)Bi_(2)I_(9)nanosheet for photocatalytic CO_(2)reduction coupled with water oxidation.The Cs_(3)Bi_(2)I_(9)/BiVO_(4)Z-scheme heterojunction photocatalyst is stable in the gas-solid photocatalytic CO_(2)reduction system,demonstrating a high visible-light-driven photocatalytic CO_(2)-to-CO production rate of 17.5μmol/(g·h),which is approximately three times that of pristine Cs_(3)Bi_(2)I_(9).The high efficiency of the Cs_(3)Bi_(2)I_(9)/BiVO_(4)heterojunction was attributed to the improved charge separation in Cs_(3)Bi_(2)I_(9).Moreover,the Z-scheme charge-transfer pathway preserves the negative reduction potential of Cs_(3)Bi_(2)I_(9)and the positive oxidation potential of BiVO_()4.This study off ers solid evidence of constructing Z-scheme heterojunctions to improve the photocatalytic performance of lead-free halide perovskites and would inspire more ideas for developing leadfree halide perovskite photocatalysts.

关键词： Lead-free halide perovskite Z-scheme heterojunction CO_(2)reduction Visible-light photocatalysis charge transfer

A Triethyleneglycol C60 Mono-adduct Derivative for Efficient Electron Transport in Inverted Perovskite Solar Cells

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Chinese Journal of Chemistry 2023年第4期41卷 431-442页

作者： Azhar Fakharuddin Konstantina-Kalliopi Armadorou Leandros P.Zorba Marinos Tountas Tobias Seewald Anastasia Soultati Polychronis Tsipas Emilia R.Schütz Nikolaos Tzoganakis Stylianos Panagiotakis Konstantina Yannakopoulou Athanasios Dimoulas Vassilis Psycharis Emmanuel Kymakis Abd Rashid bin Mohd Yusoff Konstantinos Aidinis Lukas Schmidt-Mende Georgios C.Vougioukalakis Mohammad Khaja Nazeeruddin Maria Vasilopoulou Department of Physics University of Konstanz78457 KonstanzGermany Institute of Nanoscience and Nanotechnology National Center for Scientific Research DemokritosAgia Paraskevi15341 AthensGreece Department of Chemistry National and Kapodistrian University of Athens15771 AthensGreece Department of Electrical&Computer Engineering Hellenic Mediterranean UniversityEstavromenosHeraklionGR-71410 CreteGreece Department of Chemical Engineering Pohang University of Science and Technology(POSTECH)PohangGyeongbuk37673 Republic of Korea Department of Electrical and Computer Engineering Ajman UniversityP.O.Box 346AjmanUnited Arab Emirates Center of Medical and Bio-allied Health Sciences Research AjmanUnited Arab Emirates Institute of Chemical Sciences and Engineering École Polytechnique Fédérale de Lausanne(EPFL)Rue de l'Industrie 17CH-1951 SionSwitzerland

Inverted perovskite solar cells(PSCs)have attracted increasing attention in recent years owing to their low-temperature fabrication proces s.However,they suffer from a limited number of electron transport materials available with[6,6]-phenyl C61 butyric acid methyl ester(PCBM)to be the most widely studied based on its appropriate energy levels and high electron mobility.The low relative permittivity and aggregation tendency upon illumination of PCBM,however,compromises the solar cell efficiency whereas its modest hydrophobicity negatively impacts on the device stability.Alternative electron transport materials with desired properties and appropriate degree of hydrophobicity are thus desirable for further developments in inverted PSCs.Herein,we synthesize a triethyleneglycol C60 mono-adduct derivative(termed as EPF03)and test it as a novel electron transport material to replace PCBM in inverted PSCs based on a quadruple cation(RbCsMAFA)perovskite.We also compare this derivative with two novel fullerenes decorated with two(EPF01)or one dodecyl(EPF02)long side chains.The latter two fail to perform efficiently in inverted PSCs whereas the former enabled a power conversion efficiency of 18.43%,which represents a 9%improvement compared to the reference device using PCBM(17.21%).The enhanced performance mainly stems from improved electron extraction and reduced recombination enabled by the insertion of the large relative permittivity amongst other properties of EPF03.Furthermore,our results indicate that triethylene glycol side chains can also passivate perovskite trap states,suppress ion migration and enhance photostability and long-term stability of EPF03 based perovskite solar cells.

关键词： Electron transport layer Defect passivation Biexponential trap flling charge transfer Fullerenes

Tailoring the electronic acceptor–donor heterointerface between black phosphorus and Co_(3)O_(4) for boosting oxygen bifunctional electrocatalysis

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Chinese Chemical Letters 2023年第2期34卷 284-289页

作者： Jing Zou Yilun Zou Haitao Wang Wei Wang Pingxiu Wu Arramel Jizhou Jiang Xin Li School of Chemistry and Environmental Engineering School of Environmental Ecology and Biological EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Tree Gorges LaboratoryWuhan Institute of TechnologyWuhan 430205China Key Laboratory of Rare Mineral Ministry of Natural ResourcesGeological Experimental Testing Center of Hubei ProvinceWuhan 430034China Key Laboratory of Hunan Province for Advanced Carbon-based Functional Materials Hunan Institute of Science and TechnologyYueyang 414006China Semiconductor Electronic Special Gas of Hubei Engineering Research Center Jingzhou 434000China Nano Center Indonesia Jl.PUSPIPTEK Tangerang SelatanBanten 15314Indonesia Institute of Biomass Engineering Key Laboratory of Energy Plants Resource and UtilizationMinistry of Agriculture and Rural AffairsSouth China Agricultural UniversityGuangzhou 510642China

Black phosphorus (BP) as an uprising two-dimensional material exhibits attractive potential in the field of electrocatalysis due to the inherent advantages of high carrier mobility and abundant lone pair electrons.However,the exposed active electrons compel BP to be deactivated by oxidative degradation.Herein,the electronic signature of acceptor-donor heterointerfacial interactions between BP and Co_(3)O_(4)is realized via wet ball milling.The preferential migration of active electrons from BP to Co_(3)O_(4)is achieved at the heterointerface since the Fermi level of BP is higher than that of Co_(3)O_(4).Such relative energetic consideration promotes reasonable oxygen electrocatalytic active sites.Moreover,it significantly suppresses the oxidative degradation of BP.Consequently,the resulting Co_(3)O_(4)/BP heterojunction possesses superior oxygen bifunctional electrocatalytic activity than its parent catalysts.Most importantly,this work promotes an efficient route towards BP-based multifunctional catalysts.

关键词： Electronic acceptor-donor Black phosphorus Co_(3)O_(4) charge transfer Oxygen bifunctional electrocatalysis