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Ligand-free CsPbBr_(3) with calliandra-like nanostructure for efficient artificial photosynthesis

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Journal of Energy Chemistry 2023年第2期77卷 317-325,I0009页

作者： Yan-Fei Mu Hui-Ling Liu Meng-Ran Zhang Hong-Juan Wang Min Zhang Tong-Bu Lu MOE International Joint Laboratory of Materials Microstructure Institute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009JiangsuChina

The low-efficiency CO_(2) uptake capacity and insufficient photogenerated exciton dissociation of current metal halide perovskite(MHP)nanocrystals with end-capping ligands extremely restrict their application in the field of artificial photosynthesis.Herein,we demonstrate that ligand-free CsPbBr_(3) with calliandralike nanostructure(LF-CPB CL)can be synthesized easily through a ligand-free seed-assisted dissolutionrecrystallization growth process,exhibiting significantly enhanced CO_(2) uptake capacity.More specifically,the abundant surface bromine(Br)vacancies in ligand-free MHP materials are demonstrated to be beneficial to photogenerated carrier separation.The electron consumption rate of LF-CPB CL for photocatalytic CO_(2) reduction increases 7 and 20 times over those of traditional ligand-capping CsPbBr_(3)nanocrystal(L-CPB NC)and bulk CsPbBr_(3),respectively.Moreover,the absence of ligand hindrance can facilitate the interfacial electronic coupling between LF-CPB CL and tetra(4-carboxyphenyl)porphyrin iron(Ⅲ)chloride(Fe-TCPP)cocatalyst,bringing forth significantly accelerated interfacial Charge separation.The LF-CPB CL/Fe-TCPP exhibits a total electron consumption rate of 145.6μmol g^(-1) h^(-1) for CO_(2)photoreduction coupled with water oxidation which is over 14 times higher than that of L-CPB NC/FeTCPP.

关键词： Artificial photosynthesis Charge separation Halide perovskite Ligand-free Vacancy defect

Boosting the photo-induced charge transfer in melon by lengthening the melon chains through a facile regrowth approach

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Nano Research 2023年第2期16卷 2076-2084页

作者： Tongtong Li Shulan Wang Li Li Xiaohua Yu Huaze Zhu Ningdong Feng Ju Rong Yongqiang Yang Gang Liu Department of Chemistry College of ScienceNortheastern UniversityShenyang 110819China Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of ScienceShenyang 110016China School of Metallurgy Northeastern UniversityShenyang 110819China Faculty of Materials Science and Engineering Kunming University of Science and TechnologyKunming 650093China State Key Laboratory of Magnetic Resonance and Atomic Molecular Physics Wuhan Center for Magnetic Resonance Key Laboratory of Magnetic Resonance in Biological SystemsWuhan Institute of Physics and MathematicsChinese Academy of SciencesWuhan 430071China

Melon-derived carbon nitride photocatalysts are a kind of star layered materials applied in solar energy conversion.With in-planeπorbitals of the heptazine subunits and their overlap along the melon chains being the most distinctive feature,the condition of melon chains is of great importance for the atomic and energy band structures of carbon nitride photocatalysts as well as their photo-activities.In principle,fragmentized melon chains in practical carbon nitride would lead to unfavorable structure disorder both in longitudinal and vertical directions,thus inhibiting the efficient transfer for photo-induced electrons and holes,respectively.Here,with a facile regrowth approach,that is to treat carbon nitride under the atmosphere containing C/N species,the melon chains in carbon nitride were experimentally lengthened,which was reflected by the regularly fraction variation of different nitrogen species derived from X-ray photoelectron spectroscopy(XPS)analysis.The prolonged melon chains led to dramatically improved in-plane structure order and boosted transfer of photo-induced electrons and holes,which were confirmed by the spontaneous photo-deposition of oxidants and reductants.The combination of this regrowth approach with homogenously distributed nitrogen vacancies resulted in much enhanced visible-light-responsive photoactivities.Besides,control experiments using nitrogen-vacancy-free carbon nitride and different C/N-contained precursors showed the compatibility as well as the critical factors for the lengthening effects of the regrowth approach.We hope that the facile but efficient regrowth approach could be widely adopted in melon-derived carbon nitride photocatalysts used for various applications.

关键词： carbon nitride melon chains structure order photocatalytic hydrogen evolution charge transfer Charge separation

Homojunction photocatalysts for water splitting

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Nano Research 2022年第12期15卷 10171-10184页

作者： Xiangjiu Guan Shichao Zong Shaohua Shen International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an710049China Suzhou Academy of Xi’an Jiaotong University Suzhou215123China Key Laboratory of Subsurface Hydrology and Ecological Effects in Arid Region Ministry of EducationSchool of Water and EnvironmentChang’an UniversityXi’an710064China

charge-carrier separation is regarded as one of the critical issues of photocatalytic water splitting and could be accelerated by constructing microscopic junctions in photocatalysts.Homojunction photocatalysts consisting of different forms of semiconductor with identical compositions could inherit the advantages of heterojunction-based photocatalysts in Charge separation due to the built-in electric field,while omitting the potential drawbacks of interfacial lattice distortion by providing continuous band bonding.Therefore,homojunction-based photocatalysts have recently drawn growing attention in water splitting.In this review,the synthetic approaches to preparing photocatalysts with various homojunction structures including p-n junction,phase junction,and facet junction were introduced,together with a comprehensive analysis and discussion on the latest progress in the application of photocatalytic water splitting.This review work is expected to inspire more related work with promoted research on designing efficient homojunction-based photocatalytic systems for water splitting.

关键词： photocatalytic water splitting homojunction Charge separation

Mechanism insight into the enhanced photocatalytic purification of antibiotic through encapsulated architectures coupling of crystalline Cu_(2)O/amorphous TiFe layer double hydroxide

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Journal of Materials Science & Technology 2023年第36期167卷 161-170页

作者： Lin Ye Shaodong Sun Xiaoli Yang Xiaoxi Chen Bian Yang Daqin Yun Xiaojing Yu Man Yang Qing Yang Shuhua Liang Jie Cui Engineering Research Center of Conducting Materials and Composite Technology Ministry of EducationShaanxi Engineering Research Center of Metal-Based Heterogeneous Materials and Advanced Manufacturing TechnologyShaanxi Province Key Laboratory for Electrical Materials and Infiltration TechnologySchool of Materials Science and EngineeringXi’an University of TechnologyXi’an 710048China College of Energy Xiamen UniversityXiamen 361005China

Amorphous materials are one of the important candidates for improving heterogeneous photocata-lysts because of their unique electronic structures and abundant catalytic sites originating from dis-order atomic arrangements.However,there is still much room for the development of new crys-talline/amorphous heterogeneous composites for photocatalytic application.Hence efficient synthetic strategies for preparing new crystalline/amorphous heterojunctions are highly desired.Herein,we have realized the deep optimization of photocatalytic activity by fabricating crystalline/amorphous Cu_(2)O/Ti-Fe layer double hydroxide(LDH)heterojunctions.Thanks to the typical Z-scheme mechanism originating from the crystalline/amorphous interfaces,the photoCharge separation and catalytic active sites obviously enhance compared to single Cu_(2)O and LDH counterparts.As expected,the photocatalytic removal of tetra-cycline(TC)of the as-prepared Cu_(2)O/Ti-Fe LDH was over 5.2 and 2.2 times those of the pristine Cu_(2)O nanospheres and Ti-Fe LDH nanosheets.This work illustrates the origin of crystalline Cu_(2)O nanospheres encapsulated in amorphous Ti-Fe layer double hydroxide nanosheets for enhanced photocatalytic activity driven by visible light,and provide a general Cu_(2)O-templated solution-phase synthetic method for the synthesis of novel double-metal layer double hydroxide amorphous nanostructures.

关键词： Crystalline Cu_(2)O Amorphous Ti-Fe LDH Z-scheme mechanism Charge separation Photodegradation

Accumulation of localized charge on the surface of polymeric carbon nitride boosts the photocatalytic activity

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Journal of Materials Science & Technology 2022年第16期111卷 9-16页

作者： Yabin Jiang Lei Zeng Chi Cao Wensheng Yang Limin Huang School of Materials Sun Yat-Sen UniversityShenzhen 518107China Department of Chemistry Southern University of Science and TechnologyShenzhenGuangdong 518055China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China Institute of Molecular Plus Tianjin UniversityTianjin 300072China

The random mobility of charge carriers is a main factor causing the low photocatalytic efficiency of gCN.Thus,the controllable migration of charge carriers is a rational strategy to suppress the charge recombination and facilitate Charge separation.Herein,an ethylenediamine modified g-C_(3)N_(4)displays improved photocatalytic activity.The excellent Charge separation efficiency is confirmed to be a key factor for the enhancement.The TEM observation after photo-depositing Pt nanoparticles and DFT calculations verify the accumulation of electrons on some areas of g-C_(3)N_(4)surface.The increased-NH_(2)groups significantly tune the electronic structure of g-C_(3)N_(4)after the modification.The generation of midgap states also affects the Charge separation.Our reports provide a simple method to manage the migration of charge carriers and enable electrons directional transfer,which suppresses the recombination and improves the photocatalytic activity.

关键词： g-C_(3)N_(4) Charge separation Photocatalytic H2 evolution Directional migration

Defect engineering of water-dispersible g-C_(3)N_(4) photocatalysts by chemical oxidative etching of bulk g-C_(3)N_(4) prepared in different calcination atmospheres

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Journal of Materials Science & Technology 2022年第8期103卷 232-243页

作者： Thi Kim Anh Nguyen Thanh-Truc Pham Bolormaa Gendensuren Eun-Suok Oh Eun Woo Shin School of Chemical Engineering University of UlsanDaehakro 93Ulsan 44610South Korea Department of Material Technology Faculty of Applied ScienceHo Chi Minh City University of Technology and Education(HCMUTE)No.1 Vo Van Ngan StreetLinh Chieu WardThu Duc DistrictHo Chi Minh City 700000Viet Nam

In this study,water-dispersible graphitic carbon nitride(g-C_(3)N_(4))photocatalysts were successively prepared through the chemically oxidative etching of bulk g-C_(3)N_(4) that was polymerized thermally in different calcination atmospheres such as air,CO_(2),and N_(2).The different calcination atmospheres directly influenced the physicochemical and optical properties of both bulk and water-dispersible g-C_(3)N_(4),changing the photocatalytic degradation behavior of methylene blue(MB)and tetracycline hydrochloride(TCHCl)for water-dispersible g-C_(3)N_(4).The bubble-burst process in the thermal polymerization of thiourea produced defective edges containing C=O groups that preferred substituting the C-NHx groups over bulk g-C_(3)N_(4).In the oxygen-free N_(2) atmosphere among the different calcination atmospheres,more C=O functional groups were generated on the defective edges of bulk g-C_(3)N_(4),resulting in the highest N vacancy of the tri-s-triazine structure.During the successive chemical oxidation,S-or O-containing functional groups were introduced onto water-dispersible g-C_(3)N_(4).The water-dispersible g-C_(3)N_(4) photocatalyst from the oxygen-free N_(2) atmosphere(NTw)contained the most O-and S-functional groups on the g-C_(3)N_(4) surface.Consequently,NTw exhibited the highest photocatalytic activity in the MB and TC-HCl photodegradation because of its slowest recombination process,which was ascribed to the unique surface properties of NTw such as abundant functional groups on the defective edges and N-deficient property.

关键词： g-C_(3)N_(4) Water-dispersible photocatalyst Calcination atmosphere Charge separation Chemically oxidative etching Defect edges

Constructing a coplanar heterojunction through enhancedπ-πconjugation in g-C_(3)N_(4)for efficient solar-driven water splitting

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Chinese Chemical Letters 2022年第5期33卷 2579-2584页

作者： Zihao Chen Ben Chong Nathan Wells Guidong Yang Lianzhou Wang XJTU-Oxford International Joint Laboratory for Catalysis School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an 710049China School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology the University of QueenslandQLD 4072Australia

Adjusting the electronic structure of graphitic carbon nitride(g-C_(3)N_(4))photocatalyst throughπ-πconju-gation is an effective method to achieve efficient photogenerated carrier separation.One key challenge ofπ-πconjugation control is to tune the degree of such conjugation without destroying the g-C_(3)N_(4)struc-ture.Herein we report a conceptual design that achieves a coplanar heterojunction by enhancing theπ-πconjugation via the doping of crystalline g-C_(3)N_(4)using a conjugated double bond ring molecule,1,3,5-benzenetriol,during calcination process.The selection of the dopant enables the facile creation of a unique coplanar heterojunction which not only retains the pristine network structure of g-C_(3)N_(4),but remarkably promotes separation and transfer of photogenerated carriers through the enhancedπ-conjugated endogenous electric field.As a result,the new g-C_(3)N_(4)photocatalyst efficiently photocatalyti-cally produces hydrogen from water under visible light irradiation with a high H 2 production rate up to 94.94μmol/h,and a notable external quantum efficiency of 16.4%at 420 nm.

关键词： g-C_(3)N_(4) Charge separation Coplanar heterojunction Enhancedπ-πconjugation Photocatalysis

Rational design on photoelectrodes and devices to boost photoelectrochemical performance of solar-driven water splitting: a mini review

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Frontiers of Chemical Science and Engineering 2022年第6期16卷 777-798页

作者： Siliu Lyu Muhammad Adnan Younis Zhibin Liu Libin Zeng Xianyun Peng Bin Yang Zhongjian Li Lecheng Lei Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China

As an eco-friendly,efficient,and low-cost technique,photoelectrochemical water splitting has attracted growing interest in the production of clean and sustainable hydrogen by the conversion of abundant solar energy.In the photoelectrochemical system,the photoelectrode plays a vital role in absorbing the energy of sunlight to trigger the water splitting process and the overall efficiency depends largely on the integration and design of photoelectrochemical devices.In recent years,the optimization of photoelectrodes and photoelectrochemical devices to achieve highly efficient hydrogen production has been extensively investigated.In this paper,a concise review of recent advances in the modification of nanostructured photoelectrodes and the design of photoelectrochemical devices is presented.Meanwhile,the general principles of structural and morphological factors in altering the photoelectrochemical performance of photoelectrodes are discussed.Furthermore,the performance indicators and first principles to describe the behaviors of charge carriers are analyzed,which will be of profound guiding significance to increasing the overall efficiency of the photoelectrochemical water splitting system.Finally,current challenges and prospects for an in-depth understanding of reaction mechanisms using advanced characterization technologies and potential strategies for developing novel photoelectrodes and advanced photoelectrochemical water splitting devices are demonstrated.

关键词： photoelectrochemical water splitting photoelectrodes hydrogen production Charge separation catalytic mechanism

Present and Future of Phase‑Selectively Disordered Blue TiO2 for Energy and Society Sustainability

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Nano-Micro Letters 2021年第3期13卷 53-65页

作者： Yongguang Luo Hyoyoung Lee Center for Integrated Nanostructure Physics(CINAP) Institute for Basic Science(IBS)2066 SeoburoJangan‑guSuwon 16419Republic of Korea Department of Chemistry Sungkyunkwan University2066 SeoburoJangan‑guSuwon 16419Republic of Korea Creative Research Institute(CRI) Sungkyunkwan University2066 SeoburoJangan‑guSuwon 16419Republic of Korea Department of Biophysics Sungkyunkwan University2066 SeoburoJangan‑guSuwon 16419Republic of Korea

Titanium dioxide(TiO2)has garnered attention for its promising photocatalytic activity,energy storage capability,low cost,high chemical stability,and nontoxicity.However,conventional TiO2 has low energy harvesting efficiency and Charge separation ability,though the recently developed black TiO2 formed under high temperature or pressure has achieved elevated performance.The phase-selectively ordered/disordered blue TiO2(BTO),which has visible-light absorption and efficient exciton disassociation,can be formed under normal pressure and temperature(NPT)conditions.This perspective article first discusses TiO2 materials development milestones and insights of the BTO structure and construction mechanism.Then,current applications of BTO and potential extensions are summarized and suggested,respectively,including hydrogen(H2)production,carbon dioxide(CO2)and nitrogen(N2)reduction,pollutant degradation,microbial disinfection,and energy storage.Last,future research prospects are proposed for BTO to advance energy and environmental sustainability by exploiting different strategies and aspects.The unique NPT-synthesized BTO can offer more societally beneficial applications if its potential is fully explored by the research community.

关键词： Blue TiO2(BTO) Phase-selective disordering Visible-light-driven photocatalyst Charge separation Energy and society sustainability