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Hydroxylated metal–organic-layer nanocages anchoring single atomic cobalt sites for robust photocatalytic co_(2) reduction

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Nano Research 2024年第4期17卷 2410-2419页

作者： Weiyi Pan Zhihe Wei Yanhui Su Yuebin Lian Zhangyi Zheng Huihong Yuan Yongze Qin Xulan Xie Qianqian Bai Zhenyang Jiao Wei Hua Jinzhou Chen Wenjun Yang Zhao Deng Yang Peng Soochow Institute for Energy and Materials Innovations College of EnergySoochow UniversitySuzhou 215006China Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province Soochow UniversitySuzhou 215006China School of Photoelectric Engineering Changzhou institute of technologyChangzhou 213032China Jiangsu Key Laboratory for Advanced Negative Carbon Technologies Soochow UniversitySuzhou 215123China

Assembly of two-dimensional(2D)metal–organic layers(MOLs)based on the hard and soft acid–base theorem represents an exquisite strategy for the construction of photocatalytic platforms in virtue of the highly exposed active sites,much improved mass transport,and greatly elevated stability.Herein,nanocages composed of MOLs are produced for the first time through a cosolvent approach utilizing zirconium-based UiO-66-(OH)2 as the structural precursor.To endow the catalytic activity for co_(2) conversion,single atomic co^(2+)sites are appended to the Zr-oxo nodes of the MOL cages,demonstrating a remarkable co yield of 7.74 mmol·g^(-1)·h^(-1) and operational stability of 97.1%product retention after five repeated cycles.Such an outstanding photocatalytic performance is mainly attributed to the unique nanocage morphology comprising enormous 2D nanosheets for augmented co^(2+)exposure and the abundant surface hydroxyl groups for local co_(2) enrichment.This work underlines the tailoring of both metal–organic framework(MOF)morphology and functionality to boost the turnover rate of photocatalytic co_(2) reduction reaction(co_(2)RR).

关键词： photocatalytic co_(2) reduction metal–organic layer nanocage single-atom catalyst co-catalyst

Low-dimensional MXenes as noble metal-free co-catalyst for solar-to-fuel production:Progress and prospects

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Journal of Materials Science & Technology 2022年第19期114卷 143-164页

作者： Wanying Lei Tong Zhou Xin Pang Shixiang Xue Quanlong Xu college of Materials Science and Engineering Xi’an University of Architecture and TechnologyXi’an 710055China Key laboratory of Carbon Materials of Zhejiang Province Wenzhou UniversityWenzhou 325027China

Direct conversion of solar energy into chemical fuels via semiconducting materials through photocatalytic technology is a sustainable way to tackle the global warming, environmental issue and energy crisis. Transition metal carbides and nitrides(MXenes), a newly emerging class of 2D layered materials, has gained tremendous attention as a noble metal-free co-catalyst for boosting photoreactivity due to its extraordinary characteristics like elemental abundance, excellent electrical conductivity, abundant surface functional groups, unique hydrophilic behavior and flexible modulation of chemical composition. The rational integration of low-dimensional MXenes in the form of 2D layered structures or 0D quantum dots with diverse semiconducting materials offer more versatile and robust heterostructured-photocatalysts that are applicable in solar fuel generation. Herein, we summarize the recent advances and achievements in the synthesis of low-dimensional MXenes and their application in hydrogen production from water splitting and co_(2) photoreduction. A comprehensive discussion of the fundamentals for solar fuel production, synthesis strategies and theoretical calculations for MXenes-based photocatalysts are also given. Finally, the existing challenges and further perspectives of MXenes-based nanostructures for efficient solar fuel production are addressed.

关键词： MXenes Low-dimensional materials co-catalyst Photocatalytic H_(2)evolution co_(2)photoreduction

Precise fabrication of single-atom alloy co-catalyst with optimal charge state for enhanced photocatalysis

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National Science Review 2021年第1期8卷 81-88页

作者： Yating Pan Yunyang Qian Xusheng Zheng Sheng-Qi Chu Yijun Yang Chunmei Ding Xi Wang Shu-Hong Yu Hai-Long Jiang Hefei National Laboratory for Physical Sciences at the Microscale CAS Key Laboratory of Soft Matter ChemistryDepartment of Chemistry University of Science and Technology of China National Synchrotron Radiation Laboratory (NSRL) University of Science and Technology of China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of Sciences Key Laboratory of Luminescence and Optical Information Ministry of EducationDepartment of Physics School of Science Beijing Jiaotong University Dalian National Laboratory for Clean Energy State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

While the surface charge state of co-catalysts plays a critical role for boosting photocatalysis, studies on surface charge regulation via their precise structure control remain extremely rare. Herein, metal-organic framework（MOF） stabilized bimetallic Pd@Pt nanoparticles, which feature adjustable Pt coordination environment and a controlled structure from core-shell to single-atom alloy（SAA）, have been fabricated.Significantly, apart from the formation of a Mott-Schottky junction in a conventional way, we elucidate that Pt surface charge regulation can be alternatively achieved by changing its coordination environment and the structure of the Pd@Pt co-catalyst, where the charge between Pd and Pt is redistributed. As a result, the optimized Pd;@Pt;/MOF composite, which involves an unprecedented SAA co-catalyst, exhibits exceptionally high photocatalytic hydrogen production activity, far surpassing its corresponding counterparts.

关键词： metal-organic framework (MOF) single-atom alloy (SAA) co-catalyst surface charge state photocatalysis

Improvement of photocatalytic activity of high specific surface area graphitic carbon nitride by loading a co-catalyst

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Rare Metals 2019年第5期38卷 468-474页

作者： Ye Chen Naoya Murakami Hai-Yan Chen Jia Sun Qi-Tao Zhang Zhi-Feng Wang Teruhisa Ohno Ming Zhang Department of Materials Science Faculty of EngineeringKyushu Institute of TechnologyKitakyushu 8048550Japan School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China Yangzhou Polytechnic Institute Yangzhou 225127.China Japan Science and Technology Agency Kawaguchi 3320012Japan

Graphitic carbon nitride(g-C3N4)was synthesized by heating melamine and was then treated with sodium hydroxide solution under a hydrothermal condition to obtain g-C3N4 with a large specific surface area(HSSA).HSSA shows higher photocatalytic activity for decomposition of acetaldehyde than that of original g-C3N4.HSSA was modified with RuO2 as a co-catalyst by the impregnation method.HSSA loaded with 0.05 wt%RuO2 shows the highest photocatalytic activity for acetaldehyde decomposition under visible light(k=455 nm).

关键词： Graphitic carbon nitride Organic decomposition co-catalyst Visible light

Enhanced photocatalytic N2 fixation by promoting N2 adsorption with a co-catalyst

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Science Bulletin 2019年第13期64卷 918-925页

作者： Xiang Gao Li An Dan Qu Wenshuai Jiang Yanxiao Chai Shaorui Sun Xingyuan Liu Zaicheng Sun State Key Laboratory of Luminescence and Applications Changchun Institute of OpticsFine Mechanics and PhysicsChinese Academy of SciencesChangchun 130033China University of Chinese Academy of Sciences Beijing 100190China Center of Excellence for Environmental Safety and Biological Effects Beijing Key Laboratory of Green Catalysis and Separation Department of Chemistry and Chemical EngineeringSchool of Environmental and EnergyBeijing University of TechnologyBeijing 100124China

Photocatalytic N2 fixation involves a nitrogen reduction reaction on the surface of the photocatalyst to convert N2 into ammonia.Currently,the adsorption of N2 is the limiting step for the N2 reduction reaction on the surface of the catalyst.Based on the concept of photocatalytic water splitting,the photocatalytic efficiency can be greatly enhanced by introducing a co-catalyst.In this report,we proposed a new strategy,namely,the loading of a NiS co-catalyst on CdS nanorods for photocatalytic N2 fixation.Theoretical calculation results indicated that N2 was effectively adsorbed onto the NiS/CdS surface.Temperature programmed desorption studies confirmed that the N2 molecules preferred to adsorb onto the NiS/CdS surface.Linear sweep voltammetry results revealed that the overpotential of the N2 reduction reaction was reduced by loading NiS.Furthermore,transient photocurrent and electrochemical impedance spectroscopy indicated that the charge separation was enhanced by introducing NiS.Photocatalytic N2 fixation was carried out in the presence of the catalyst dispersed in water without any sacrificial agent.As a result,1.0 wt% NiS/CdS achieved an ammonia production rate of 2.8 and 1.7 mg L-1 for the first hour under full spectrum and visible light(λ>420 nm),respectively.The catalyst demonstrated apparent quantum efficiencies of 0.76%,0.39% and 0.09% at 420,475 and 520 nm,res pectively.This study provides a new method to promote the photocatalytic efficiency of N2 fixation.

关键词： N2 fixation Photocatalyst co-catalyst N2 adsorption NiS

Improved Oxygen Evolution Kinetics and Surface States Passivation of Ni-Bi co-catalyst for a Hematite Photoanode

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Engineering 2017年第3期3卷 285-289页

作者： Ke Dang Tuo Wang Chengcheng Li Jijie Zhang Shanshan Liu Jinlong Gong Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and Technology Tianjin University. Tianjin 300072 China collaborative Innovation Center of Chemical Science and Engineering Tianjin 300072 China

This paper describes the combinational surface kinetics enhancement and surface states passivation of nickel-borate (Ni-Bi) co-catalyst for a hematite (Fe2O3) photoanode. The Ni-Bi-modified Fe2O3 photoanode exhibits a cathodic onset potential shift of 230 mV and a 2.3-fold enhancement of the photocurrent at 1.23 V, versus the reversible hydrogen electrode (RHE). The borate (Bi) in the Ni-Bi film promotes the release of protons for the oxygen evolution reaction (OER).

关键词： Nickel-borate Hematite Oxygen evolution reaction co-catalyst

The effect of co-catalysts on the morphology of isotactic polypropene prepared using metallocene catalyst

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Chinese Science Bulletin 2002年第10期47卷 810-813页

作者： ZHANG Mingge XU Demin HONG Han GUO Cunyue HU Youliang State Key Lab of Engineering Plastics Center for Molecular ScienceInstitute of ChemistryChinese Academy of SciencesBeijing Lab of CatalysisKey Lab ot Catalysis of China National Petroleum CorporationBeijing 100080China Graduate School of the Chinese Academy of Sciences Beijing 100030China

SiO2/rac-Me2Si[2-Me-4-Naph-Ind]2ZrCl2 was prepared and different co-catalysts were used in bulk polymerization of propene. The morphology of polypropene could be controlled by altering the co-catalysts. The isotactic polypropene with good morphology and high bulk density were prepared. The formation mechanism of active centers was proposed, by which the effect of co-catalysts on the morphology of polypeopene was analyzed.

关键词： metallocene co-catalyst supporting morphology of polypropene.

Effects of Bi-dopant and co-catalysts upon hole surface trapping on La_(2)Ti_(2)O_(7) nanosheet photocatalysts in overall solar water splitting

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Nano Research 2022年第1期15卷 438-445页

作者： Xiaoyan Cai Liang Mao Mamoru Fujitsuka Tetsuro Majima Sujan Kasani Nianqiang Wu Junying Zhang School of Materials Science and Physics Jiangsu Province Engineering Laboratory of High Efficient Energy Storage Technology and EquipmentChina University of Mining and TechnologyXuzhou 221116China School of Physics Beihang UniversityBeijing 100191China The Institute of Scientific and Industrial Research(SANKEN) Osaka UniversityMihogaoka 8-1IbarakiOsaka 567-0047Japan Department of Mechanical and Aerospace Engineering West Virginia UniversityMorgantownWV 26506-6106USA Department of Chemical Engineering University of Massachusetts AmherstAmherstMA 01003-9303USA

Pristine and Bi-doped lanthanum titanium oxide(La_(2)Ti_(2)O_(7))nanosheets have been synthesized as photocatalysts for overall solar water splitting.The surface hole trap is a critical factor that limits the photocatalytic activity of pristine La_(2)Ti_(2)O_(7)-Deposition of cobalt phosphate(co-Pi)and platinum(Pt)nanoparticles on La_(2)Ti_(2)O_(7) cannot remove the surface traps although they are essential for enabling the oxygen and hydrogen evolution reactions.It is interesting that doping bismuth(Bi)into La_(2)Ti_(2)O_(7) nanosheets has eliminated the surface traps due to surface enrichment of Bi.The co-Pi/Bi-La_(2)Ti_(2)O_(7)/Pt nanosheets exhibit increasing photocatalytic activity toward overall water splitting with increasing the Bi-dopant level up to 5 at.%.Further increasing the Bi-dopant level leads to the formation of localized states above the valence band,leading to the lifetime reduction of photogenerated charge-carriers,and jeopardizing the photocatalytic activity.This work proposes an effective strategy to address the surface trapping and surface catalysis issues in the nanostructured metal oxide photocatalysts.

关键词： photocatalyst water splitting surface trap co-catalyst solar fuel

Pt-surface oxygen vacancies coupling accelerated photo-charge extraction and activated hydrogen evolution

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Nano Research 2023年第4期16卷 4736-4741页

作者： Fangxu Dai Mingming Zhang Mingzhong Mi Zhenjiang Li Jun Xing Lei Wang Key Laboratory of Eco-chemical Engineering Ministry of EducationCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China college of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China college of Environment and Safety Engineering Qingdao University of Science and TechnologyShandong Engineering Research Center for Marine Environment Corrosion and Safety ProtectionQingdao 266042China

Semiconductors-based heterogeneous photocatalytic water splitting has been extensively studied,but it still remains challenging to accelerate the separation of electron-hole pairs and facilitate the reaction kinetics.Here we report a general strategy to fabricate highly efficient Pt/TiO_(2)photocatalyst by coupling the Pt co-catalysts and surface oxygen vacancies(VO)of TiO_(2).TiO_(2)was pre-modified with alkali or alkaline earth metals ion solutions,which produce a large number of surface hydroxyl on TiO_(2).Subsequently,the photodeposited Pt sub-nanoparticles substitute surface hydroxyl and induce surface VO on TiO_(2).The coupling of Pt and surface VO on TiO_(2)can accelerate the extraction of photo-charges through the interaction of Pt-VO-Ti bonds and reduce the hydrogen evolution barrier,thereby promoting the photocatalytic activity.The synthesized Pt-VO-TiO_(2)sample exhibits a photocatalytic hydrogen evolution activity as high as 1.5 L·g^(−1)·h^(−1),which is 2.2 times that of traditional Pt/TiO_(2).Our findings indepth understand the synergistic effect of co-catalysts and defects on photocatalysis and open up new possibilities for achieving robust photocatalytic water splitting.

关键词： oxygen vacancies co-catalyst surface hydroxyl photocatalytic hydrogen evolution reaction(HER)