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Mesoporous TiO_2/Carbon Beads: One-Pot Preparation and Their Application in Visible-Light-Induced Photodegradation

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Nano-Micro Letters 2015年第3期7卷 243-254页

作者： Xiaowei Li Yanqiu Jiang Wenjing Cheng Yudong Li Xianzhu Xu kaifeng lin Academy of Fundamental and Interdisciplinary Sciences Harbin Institute of Technology

Mesoporous Ti O2/Carbon beads have been prepared via a facile impregnation-carbonization approach, in which a porous anion-exchange resin and K2 Ti O(C2O4)2were used as hard carbon and titanium source, *** results reveal that the self-assembled composites have disordered mesostructure, uniform mesopores,large pore volumes, and high surface areas. The mesopore walls are composed of amorphous carbon, well-dispersed and confined anatase or rutile nanoparticles. Some anatase phase of Ti O2 was transformed to rutile phase via an increase of carbonization temperature or repeated impregnation of the resin with Ti O(C2O4)22-species. X-ray photoelectron spectroscopy, carbon, hydrogen, and nitrogen element analysis, and thermal gravity analysis results indicate the doping of carbon into the Ti O2 lattice and strong interaction between carbon and Ti O2 nanoparticles. A synergy effect by carbon and Ti O2 in the composites has been discussed herein on the degradation of methyl orange under visible light. The dye removal process involves adsorption of the dye from water by the mesopores in the composites, followed by photodegradation on the separated dye-loaded catalysts. Mesopores allow full access of the dye molecules to the surface of Ti O2 ***, the bead format of such composite enables their straightforward separation from the reaction mixture in their application as a liquid-phase heterogeneous photodegradation catalyst.

关键词： Ti O2nanoparticles Mesoporous carbon Composite bead Visible light Easy separation

Heat diffusion optimization in high performance perovskite solar cells integrated with zeolite

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Journal of Energy Chemistry 2023年第11期86卷 308-317,I0007页

作者： Wei Wang Jian Zhang kaifeng lin Jiaqi Wang Boyuan Hu Yayu Dong Debin Xia Yulin Yang MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina

Heat accumulation inside perovskite solar cells causes the decomposition of the perovskite layer and hole transport materials(HTMs)under working conditions,yielding a decrease in long-term ***,we present a zeolite-assisted heat conduction strategy by introducing economic zeolite crystals(e.g.,NaX,NaY,and ZSM-5)as a cooling filter to induce heat *** fitted thermal diffusion kinetic equation from real-time infrared thermal imaging technology reveals the zeolite skeleton assisted thermal co nduction mechanism of internal lattice ***,the nearly twofold improved conductivity of the modified HTM film is benefited from Na^(+)hopping on the supercages of the zeolite,therefore,the best-performed device with a rapid heat diffusion and defect inhibition obtains a remarkable power conversion efficiency of 23.42%.Both of NaX modified sprio-OMeTAD and PTAA based devices exhibit excellent operational stability after heating 1000 h at 85℃under N_(2)*** work demonstrates the potential application of economical porous zeolite materials in improving the thermal stability of PSCs.

关键词： Zeolite Heat diffusion Perovskite solar cells Operational stability

A-site assisted perovskite crystallization via ion-exchange MOFs for high efficient and stable perovskite solar cells

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Journal of Energy Chemistry 2024年第6期93卷 436-442,I0011页

作者： Xingrui Zhang Jian Zhang Wei Wang Boyuan Hu Yayu Dong Debin Xia kaifeng lin Yulin Yang MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina

Here,a novel strategy is proposed targeting the volatility of A-site cations and the disordered arrangement of perovskite grains through employing Cs~+contained metal-organic frameworks In-aip(Cs)obtained by ion-exchange and crystalline *** forces between Cs-O atoms split the pore channels of the pristine In-aip,endowing In-aip(Cs)with multidimensional charge transport channels,In addition,the partially freed Cs~+in the interlayer compensates for the vacancy of A-site cations during the perovskite preparation *** In-aip(Cs)modified perovskite films have a flat morphology,large grains and excellent optoelectronic *** from the high-quality perovskite films and faster charge extraction,the In-aip(Cs)-modified PSCs achieved a champion PCE of 23.03%,superior to the In-aip-modified(22.29%)and control device(21.13%),More importantly,the unencapsulated PSCs modified with In-aip(Cs)exhibited outstanding humidity and thermal *** a period of almost 1000 h,the unencapsulated In-aip(Cs)-modified device retained 85%of its initial PCE after storing in a glove box at 85℃,and retained 87%of the primary PCE upon storage in ambient condition at 25℃under a humidity of 40%.

关键词： Metal-organic frameworks PSCs Stability Defect passivation

Easily Separated and Recyclable Amino-functionalized Porous SiO2 Beads with 3D Continuous Meso/Macropore Channels

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Chemical Research in Chinese Universities 2018年第1期34卷 13-18页

作者： WANG Qi YANG Xiaohui JIANG Yanqiu HUO Hang LI Defeng lin kaifeng XU Xianzhu MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin lnstimte of Technology Harbin 150090 P. R. China Key Laboratory of Advanced Energy Materials Chemistry Ministry of Education Nankai University Tianjin 300071 P. R. China

Amino-fimctionalized porous SiO2 beads with a diameter of 200--800 μm（PSB-NH2） have been success- fully synthesized by grafting 3-ammopropyl-triethoxysilane onto meso/macroporous silica beads（PSB）, in which the PSB was prepared by hydrothermal synthetic method with a porous hard template anion-exchange resin. The as-prepared materials were characterized by means of nitrogen sorption and transmission electron micrographs（TEM）, showing the presence of 3D interconnected and continuous large mesopores and macropores inside. The beads were used to catalyze Knoevenagel condensation and proved to be highly active and selective due to the high accessibility of the reactants to the amino groups via the continuous 3D meso/macopores. Notably, such material in bead format facilitates the extremely straightforward separation from reaction solution without any centrifugation or filtration. Moreover, PSB-NH2 proved to be a stable catalyst via leaching experiment test, and can be easily recovered and reused without significant loss of activity in successive catalytic cycles.

关键词： Amino group, Porous SiO2 bead, Continuous 3D meso/macropore Knoevenagel condensation Straightforward separation

In Situ Preparation and Analysis of Bimetal Co?doped Mesoporous Graphitic Carbon Nitride with Enhanced Photocatalytic Activity

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Nano-Micro Letters 2019年第1期11卷 175-190页

作者： Wanbao Wu Zhaohui Ruan Junzhuo Li Yudong Li Yanqiu Jiang Xianzhu Xu Defeng Li Yuan Yuan kaifeng lin School of Chemistry and Chemical Engineering Harbin Institute of Technology Key Laboratory of Aerospace Thermophysics Ministry of Industry and Information TechnologyHarbin Institute of Technology

A novel photocatalyst of mesoporous graphitic carbon nitride(g-C_3N_4) co-doped with Co and Mo(Co/Mo-MCN) has been one-pot synthesized via a simple template-free method; cobalt chloride and molybdenum disulfide were used as the Co and Mo sources, respectively. The characterization results evidently indicate that molybdenum disulfide functions as Mo sources to incorporate Mo atoms in the framework of g-C_3N_4 and as a catalyst for promoting the decomposition of g-C_3N_4, resulting in the creation of mesopores. The obtained Co/Mo-MCN exhibited a significant enhancement of the photocatalytic activity in H_2 evolution(8.6 times) and Rhodamine B degradation(10.1 times) under visible light irradiation compared to pristine g-C_3N_4. Furthermore, density functional theory calculations were applied to further understand the photocatalytic enhancement mechanism of the optical absorption properties at the atomic level after Co-or Mo-doping. Finite-di erence time-domain simulations were performed to evaluate the e ect of the mesopore structures on the light absorption capability. The results revealed that both the bimetal doping and the mesoporous architectures resulted in an enhanced optical absorption; this phenomenon was considered to have played a critical role in the improvement in the photocatalytic performance of Co/Mo-MCN.

关键词： Co-doped g-C3N4 Porous g-C3N4 Photocatalysis Optical simulation Light absorption intensity

Side chain modulated ferrocene derivative as the interstitial conductive medium for high-performance and stable perovskite solar cells

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Journal of Energy Chemistry 2024年第11期98卷 645-655页

作者： Boyuan Hu Jian Zhang Yulin Yang Yayu Dong Jiaqi Wang Wei Wang Xingrui Zhang kaifeng lin Debin Xia MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina School of Materials Science and Engineering East China Jiaotong UniversityNanchang 330013JiangxiChina

The interfacial nonradiative recombination loss caused by the deep traps and mismatched band alignment restrained the commercial viability of perovskite solar cells(PSCs). Herein, we have constructed ferrocene carboxylic acid(FcA) and octafluoropentyl-ferrocenyl-carboxylate(OFFcA) interstitial conductive mediums to modulate the integral heterointerface properties and the photovoltaic performances of *** comparing the passivation strengths of the two molecules, we found that the synergistic effects among Fc/Fc^(+)redox shuttle, C=O group, and F substituents realize the optimal elimination of interfacial trap sources. Electron-withdrawing F groups reinforce the capacity of the Fc/Fc^(+)redox shuttle for the healing of metallic Pb defects and provide extensive anchoring sites to stabilize the organic ***, the homogeneity of the OFFcA layer as well as the humidity stability of perovskite film are facilitated through the introduction of F substituents, which reduce the contact resistance and improve the interfacial charge transfer. The champion OFFcA-modified device delivers an exceptional PCE of 23.62%, exceeding those of the control(PCE=22.32%) and FcA-modified(PCE=23.06%) ***, the unencapsulated OFFcA-modified device retains 82.7% of the primary efficiency at 60%RH for more than 50 d and only loses less than 10% of the primary efficiency when stored in a glove box for more than 2000 h.

关键词： Perovskite solar cells Heterointerface energetic Defect elimination Synergistic effect Stability

Dual-functional POM@IL complex modulate hole transport layer properties and interfacial charge dynamics for highly efficient and stable perovskite solar cells

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Chinese Chemical Letters 2024年第7期35卷 461-464页

作者： Boyuan Hu Jian Zhang Yulin Yang Yayu Dong Jiaqi Wang Wei Wang kaifeng lin Debin Xia MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China

The severe interfacial charge recombination as well as the stability issues brought by the Li-TFSI still hinder the commercialization of high-performance perovskite solar cells(PSCs).Here,a polyoxometalates(POMs)-based complex,POM@ionic liquid(IL),is synthesized and applied as an effective additive that simultaneously enhances the performance and stability of *** interactions between POM@IL complex and Li-TFSI inhibit the aggregation of *** synergistic oxidation of POM@IL complex and Li-TFSI towards 2,2,7,7-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene(Spiro-OMeTAD)effectively enhances the electrical properties of hole transport layer film and the photovoltaic performances of *** champion device modified with the POM@IL complex yields an excellent power conversion efficiency(PCE)of 22.73%.Moreover,the incorporation of POM@IL improves the humidity stability of *** storing under high humidity conditions(25℃,60%RH)for 1200 h,the POM@IL modified device retained a remarkable 81.2%of its initial *** work provides new insight into constructing POMs-based materials for high-performance photovoltaic devices.

关键词： Polyoxometalates Ionic liquid Perovskite solar cells Energy alignment Humidity stability

Benzothiophene and benzosulfone fused pyrazino[2,3-g]quinoxaline:Synthesis and semiconducting properties

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Chinese Chemical Letters 2023年第2期34卷 563-566页

作者： Fangwei Ding Debin Xia Xiping Ding Ruibin Deng Congwu Ge Yulin Yang Ruiqing Fan kaifeng lin Xike Gao MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Shanghai Institute of Organic Chemistry Chinese Academy of SciencesShanghai 200032China

A novel air-stable n-type benzothiaphene endcapped azaarene(BTPQ) and its sulfonated derivative(BSPQ) were prepared via two pathways and characterized by NMR, UV–vis, fluorescence and cyclic voltammetry spectroscopy. Symmetrically introducing four nitrogen atoms into acenes, the semiconductor properties could be changed from p-type to n-type detected through the space charge limited current(SCLC) method. After sulfonation of BTPQ, BSPQ is with deeper frontier orbital energy levels and enhanced the electron mobility.

关键词： Azaarenes Deep LUMO levels n-type Organic semiconductor Polycyclic aromatic hydrocarbons

Multifunctional MOF@COF Nanoparticles Mediated Perovskite Films Management Toward Sustainable Perovskite Solar Cells

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Nano-Micro Letters 2024年第9期16卷 195-208页

作者： Yayu Dong Jian Zhang Hongyu Zhang Wei Wang Boyuan Hu Debin Xia kaifeng lin lin Geng Yulin Yang MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangPeople’s Republic of China School of Materials Science and Engineering East China Jiaotong UniversityNanchang 330013JiangxiPeople’s Republic of China School of Materials Science and Engineering Harbin Institute of TechnologyHarbin 150001HeilongjiangPeople’s Republic of China

Although covalent organic frameworks(COFs)with highπ-conjugation have recently exhibited great prospects in perovskite solar cells(PSCs),their further application in PSCs is still hindered by face-to-face stacking and aggregation ***,metal-organic framework(MOF-808)is selected as an ideal platform for the in situ homogeneous growth of a COF to construct a core-shell MOF@COF nanoparticle,which could effectively inhibit COF stacking and *** synergistic intrinsic mechanisms induced by the MOF@COF nanoparticles for reinforcing intrinsic stability and mitigating lead leakage in PSCs have been *** complementary utilization ofπ-conjugated skeletons and nanopores could optimize the crystallization of large-grained perovskite films and eliminate *** resulting PSCs achieve an impressive power conversion efficiency of 23.61%with superior open circuit voltage(1.20 V)and maintained approximately 90%of the original power conversion efficiency after 2000 h(30-50%RH and 25-30℃).Benefiting from the synergistic effects of the in situ chemical fixation and adsorption abilities of the MOF@COF nanoparticles,the amount of lead leakage from unpackaged PSCs soaked in water(<5 ppm)satisfies the laboratory assessment required for the Resource Conservation and Recovery Act Regulation.

关键词： Perovskite solar cells Covalent organic frameworks Metal-organic frameworks Lead leakage Stability