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SSRN 2022年

作者： Zhang, Jingtao Zeng, Dongni Xu, Changfu Hu, Wenchao Liu, Peng Cao, Shaowen Chen, Ying School of Materials and Energy Guangdong University of Technology Guangzhou510006 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China

Exploiting large-size monolithic semiconductor photocatalyst sheet/layer with superior photocatalytic hydrogen production performances through facile and scalable methods is an important research direction in promoting the practical application of traditional particulate semiconductor photocatalyst, yet challenging. Here we constructed an amorphous MoSx - CdS monolithic heterostructured photocatalyst sheet (a-MoSx - CdS/Ti) with maximal size of ~100 cm2 through a one-step potentiostatic electrodeposition process of 5 minutes on titanium mesh used as photocatalyst support. Owing to synergic effects of favorable light absorption, abundant active sites for proton reduction, effective photogenerated charge separation and robust structural integrity, the a-MoSx - CdS/Ti not only exhibits an optimized H2 generation rate of 4476 μmol h−1 g−1, but also demonstrates excellent operability during photocatalytic H2 generation and subsequent recycling processes, greatly improving its applicability. This work presents a straightforward and practical route to produce efficient, robust and easily operable photocatalytic H2 production system which expectantly finds promising practical applications in photocatalysis, photoelectrocatalysis and beyond. © 2022, The Authors. All rights reserved.

关键词： Cadmium sulfide

Cellulose Composite Kvo Films and Self-Healing Loc Gel Electrolyte for Multifunctional Flexible Electrochromic Device

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SSRN 2023年

作者： Sun, Shuokun Xia, Xiaoyan Gao, Mingrui Wei, Wei Cui, Shichuang Zhu, Quanyao School of Materials Science and Engineering Wuhan University of Technology Hubei Wuhan430070 China State Key Laboratory of Advanced Technology For Materials Synthesis and Processing Hubei Wuhan430070 China Department of Physics Changji University Xinjiang Changji831100 China

Electrochromic materials have attracted intensive attention due to friendly relationship to the environment, energy and user experience. Layered vanad-based compounds are considered as one kind of the most promising electrochromic materials. However, they are plagued by the appearance of ion channel collapse, capacity loss, and aqueous electrochromic materials exhibit poor cycling stability. Herein, we report on KV3O8·0.75H2O (KVO) and further complexed it into a network formed by linear methylcellulose, realizes a stand-alone cellulose composite KVO electrochromic film. K doping destroys the preferred orientation of V2O5 (002) crystal plane and expands the interplanar spacing to 6.9 Å. Cellulose significantly increases the viscosity of the sol (6 times) and acts as a "strengthener". Firstly, the electrochromic properties of methylcellulose composite KVO film (KVO/MC) were studied in 1 mol L-1 LiClO4 nonaqueous electrolyte. The film can freely switch between green-yellow and orange-red, and can retain more than 67% of the charge capacity after 2000 cycles. We further introduce flexible electrochromic devices assembled from KVO/MC films. Development of a self-healing LOC-based gel electrolyte composed of Ethene, 1-chloro-1,2,2-trifluoro-, polymer with 1,1- difluoroethene (P(CTFE-VDF)) and Li+ electrolyte, which is highly consistent with the device. It has a high colouring efficiency of 78.8 cm2 C -1 , achieving fast response (≤5.6 s) and long service life (>77% of the charge capacity and 70% of the optical contrast after 10000 cycles). This design shows great application potential in manufacturing large-area (20×30 cm2 ) flexible devices. © 2023, The Authors. All rights reserved.

关键词： Electrochromism

H2O molecule adsorption on s-triazine-based g-C3N4

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Chinese Journal of Catalysis 2021年第1期42卷 115-122页

作者： Bicheng Zhu Liuyang Zhang Bei Cheng Yan Yu Jiaguo Yu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina Key Laboratory of Eco-materials Advanced Technology College of Materials Science and EngineeringFuzhou UniversityFuzhou 350116FujianChina School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina

The interaction between a gas molecule and photocatalyst is vital to trigger photocatalytic *** surface state of photocatalyst affects much in this ***,adsorption of H2O molecules on s-triazine-based g-C3N4 was thoroughly studied by first-principle *** various initial adsorption models with multifarious locations of H2O molecules were built,the optimized models with strong adsorption energy pointed to the same adsorption configuration,in which the H2O molecule hold an upright orientation above the corrugated g-C3N4 *** intermolecular O-H…N hydrogen bond formed via the binding of a polar O-H bond in H2O molecule and a two-coordinated electron-rich nitrogen atom in *** the bridging effect of this intermolecular hydrogen bond,electrons would transfer from g-C3N4 to the H2O molecule,thereby lowering the Fermi level and enlarging work function of ***,regardless of the substitute,i.e.g-C3N4 multilayer,large supercell and nanotube,this adsorption system was highly reproducible,as its geometry structure and electronic property remained *** addition,the effect of nonmetal element doping on adsorption energy was *** work not only disclosed a highly preferential H2O adsorbed g-C3N4 architecture established by intermolecular hydrogen bond,but also contributed to the deep understanding and optimized design in water-splitting process on g-C3N4-based photocatalysts.

关键词： g-C3N4 H2O Density functional theory Hydrogen bond Adsorption energy

Scalable fabrication and active site identification of MOF shell-derived nitrogen-doped carbon hollow frameworks for oxygen reduction

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Journal of materials Science & technology 2021年第7期66卷 186-192页

作者： Jiashen Meng Ziang Liu Xiong Liu Wei Yang Lianzhou Wang Yan Li Yuan-Cheng Cao Xingcai Zhang Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan430070China Nanomaterials Centre School of Chemical Engineering and Australian Institute for Bioengineering and NanotechnologyThe University of QueenslandSt LuciaQLD4072Australia Shenzhen Power Supply Col.Ltd. Shenzhen CityChina State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan430074China John A.Paulson School of Engineering and Applied Sciences Harvard UniversityCambridgeMA02138United States

Nitrogen-doped carbon materials as promising oxygen reduction reaction(ORR) electrocatalysts attract great interest in fuel cells and metal-air batteries because of their relatively high activity, high surface area, high conductivity and low cost. To maximize their catalytic efficiency, rational design of efficient electrocatalysts with rich exposed active sites is highly desired. Besides, due to the complexity of nitrogen species, the identification of active nitrogen sites for ORR remains challenging. Herein, we develop a facile and scalable template method to construct high-concentration nitrogen-doped carbon hollow frameworks(NC), and reveal the effect of different nitrogen species on theirORRactivity on basis of experimental analysis and theoretical calculations. The formation mechanism is clearly revealed, including low-pressure vapor superassembly of thin zeolitic imidazolate framework(ZIF-8) shell on ZnO templates,in situ carbonization and template removal. The obtained NC-800 displays better ORR activity compared with other NC-700 and NC-900 samples. Our results indicate that the superior ORR activity of NC-800 is mainly attributed to its content balance of three nitrogen species. The graphitic N and pyrrolic N sites are responsible for lowering the working function, while the pyridinic N and pyrrolic N sites as possible active sites are beneficial for increasing the density of states.

关键词： MOF shell Nitrogen-doped carbon Hollow framework Oxygen reduction Active nitrogen sites

Bimetal-organic framework-derived carbon nanocubes with 3D hierarchical pores as highly efficient oxygen reduction reaction electrocatalysts for microbial fuel cells

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Science China materials 2021年第12期64卷 2926-2937页

作者： Neng Chen Zihan Meng Rui Wang Shichang Cai Weibin Guo Haolin Tang Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory Xianhu Hydrogen ValleyFoshan 528200China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Noble metal-free and highly efficient electrocatalytic materials with hierarchically porous structures continue to be studied for the oxygen reduction reaction(ORR) in microbial fuel cells(MFCs). We report bimetal-organic framework(bi-MOF)-derived nanocubic Swiss cheese-like carbons with a novel three-dimensional hierarchically porous structure(3D Co-N-C) prepared by utilizing cetyltrimethylammonium bromide(CTAB) as a structure-directing agent to control the formation of a nanocubic skeleton, and silica spheres as a template to form a mesoporous structure. The elemental composition and chemical morphology of this material can be tuned through the Zn/Co ratio to optimize its ORR catalytic activity. The optimized 3D Co-N-C displays excellent ORR catalytic performance(half-wave potential as high as 0.754 V vs. reversible hydrogen electrode and diffusion-limiting current density of 5.576 mA cm^(-2)) in 0.01 mol L^(-1) phosphate-buffered saline(PBS electrolyte),showing it can compete with the commercial 20 wt% Pt/C catalysts. The catalytic capability and long-term durability of 3D Co-N-C as an air-filled cathode electrocatalyst in an MFC device are tested, showing that the 3D CoNC-MFC can reach a high power density of 1257 mW m^(-2) and provide a competitive voltage during a periodic feeding operation for 192 h;these values are much higher than those of the Pt/C-MFC.

关键词： Co-N-doped carbon structure-oriented approach 3D hierarchically porous nanocubes oxygen reduction reaction microbial fuel cells

Microstructure and Oxidation Resistance of V Thin Films Deposited by Magnetron Sputtering at Room Temperature

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Journal of Wuhan University of technology(materials Science) 2020年第5期35卷 879-884页

作者： ZHANG Song ZHANG Ziyu LI Jun TU Rong SHEN Qiang WANG Chuanbin LUO Guoqiang ZHANG Lianmeng State Key Laboratory of Advanced Technology for Materials Synthesis and ProcessingWuhan University of TechnologyWuhan 430070China National Key Laboratory for Shock Wave and Detonation Physics Institute of Fluid PhysicsMianyang 621900China

Vanadium films were deposited on Si(100)substrates at room temperature by direct current(DC)magnetron *** microstructure and surface morphology were studied using scanning electron microscopy(SEM)and atomic force microscope(AFM).The oxidation resistance of films in air was studied using X-ray photoelectron spectroscopy(XPS)and transmission electron microscopy(TEM).The results showed that the amorphous vanadium film with a flatter surface had higher oxidation resistance than the crystalline film when exposed to *** rapid formation of the thin oxide layer of amorphous vanadium film could protect the film from sustained oxidation,and the relative reasons were discussed.

关键词： vanadium films magnetron sputtering sputtering power(Ps) microstructure oxidation resistance

Polyimide-Coated Mgo Nanoparticles Improves High-Temperature Energy Storage Performance in Polyetherimide-Based Nanocomposite Films

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SSRN 2024年

作者： Chen, Ying Yu, Tianjiao Chang, Xiangwu Guo, Zongqiang Zhao, Zihan Huang, Ziyue Hu, Penghao State Key Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing100084 China Institute for Advanced Materials & Technology University of Science & Technology Beijing Beijing100083 China Institute for New Materials Foshan528200 China

Enhancing the energy storage capacity of dielectric polymers can be achieved by the introduction of inorganic nanoparticles. However, the difference in surface energy often influences the interfacial compatibility of nanoparticles with polymers, consequently limiting their comprehensive dielectric properties. Here, the magnesium oxide (MgO) nanoparticles were coated with polyimide (PI) shells via in-situ polymerization, which is beneficial to improve the scattered particles in the polyether imide (PEI) matrix. The PI buffer shell is tightly bound to the PEI matrix through automatic electrostatic interaction making the defects decrease, together with the increased dielectric permittivity (Εr) attributed to MgO, significantly enhancing the discharged energy density (Udis) and storage efficiency (η) of the PI@MgO/PEI nanocomposite films in harsh conditions. Thus, the maximal Udis of the PI@MgO/PEI nanocomposites is 4.33 J/cm3 at 150 °C, twice that of the pristine PEI. Even if an η exceeds 90%, the Udis of 3.83 J/cm3 of 1 vol%-PI@MgO/PEI at 500 MV/m and 150 °C is better than that of the most advanced dielectric polymers. © 2024, The Authors. All rights reserved.

关键词： Polymer matrix composites

Enhancing the Humidity Resistance of Perovskite Photovoltaics: Comprehensive PbI2 Management Utilizing Long-Chain Ionic Liquid

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SSRN 2024年

作者： Sun, Yonggui Wang, Fei Lu, Lu Wang, Taomiao Yang, Guo Liang, Xiao Zhou, Xianfang Sun, Xiaokang Li, Qiannan Li, Yongjun Zhang, Fan Duan, Dawei Zhu, Jiajie Zhu, Quanyao Hu, Ruiyuan Yuan, Mingjian Hu, Hanlin Hoffmann Institute of Advanced Materials Shenzhen Polytechnic University 7098 Liuxian Boulevard Shenzhen518055 China Nanjing University of Posts and Telecommunications Nanjing210023 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and Engineering Wuhan University of Technology Wuhan China Shenzhen University China College of Chemistry Nankai University Tianjin China

Effectively managing residual PbI2 in two-step perovskite fabrication, while simultaneously enhancing the device performance, especially its humidity stability, poses a significant challenge. Herein, we introduced a novel ionic liquid (IL) molecule, long-chain alkane-based 1-octyl-3-methylimidazolium chloride (OMIMCl), with excellent hydrophobicity to regulate the perovskite conversion process, aiming to enhance the performance of resulting perovskite solar cells. The introduction of OMIMCl contributes to the formation of a uniform porous PbI2 film, facilitating comprehensive penetration of the second-step organic salt to fully convert PbI2 into perovskite material. Interestingly, nearly no residual PbI2 clusters are observed at both the top and bottom surfaces of OMIMCl-modified perovskite films. Meanwhile, depth-resolved grazing incidence wide-angle x-ray scattering (GIWAXS) measurements have quantitatively demonstrated the reduction of PbI2 in OMIMCl-modified perovskite thin films. Notably, the incorporation of OMIMCl retards the growth rate of perovskite crystals efficiently, thereby assisting in generating high-quality of perovskite films with larger grain size. Moreover, density functional theory (DFT) calculations of binding energy numerically demonstrate the hydrophobic property of IL OMIMCl, which plays a crucial role in improving the humidity stability of PSCs, as evidenced by direct water-dipping test. Consequently, we achieved a champion power conversion efficiency (PCE) of 24.72% and significantly improved long-term stability. © 2024, The Authors. All rights reserved.

关键词： Lead compounds

Single copper sites dispersed on hierarchically porous carbon for improving oxygen reduction reaction towards zinc-air battery

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Nano Research 2021年第4期14卷 998-1003页

作者： Wenjie Wu Yan Liu Dong Liu Wenxing Chen Zhaoyi Song Ximin Wang Yamin Zheng Ning Lu Chunxia Wang Junjie Mao Yadong Li State Key Laboratory of Heavy Oil Processing College of New Energy and MaterialsChina University of PetroleumBeijing 102249China Key Laboratory of Functional Molecular Solids Ministry of EducationAnhui Province Key Laboratory of Optoelectric Materials Science and Technology and Anhui Laboratory of Molecule-Based MaterialsAnhui Normal UniversityWuhu 241002China State key Lab of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Department of Chemistry Tsinghua UniversityBeijing 100084China

The demand for high-performance non-precious-metal electrocatalysts to replace the noble metal-based catalysts for oxygen reduction reaction(ORR)is intensively ***,single-atomic copper sites supported on N-doped three-dimensional hierarchically porous carbon catalyst(Cu_(1)/NC)was prepared by coordination pyrolysis ***,the Cu_(1)/NC-900 catalyst not only exhibits excellent ORR performance with a half-wave potential of 0.894 V(***)in alkaline media,outperforming those of commercial Pt/C(0.851 V)and Cu nanoparticles anchored on N-doped porous carbon(CuNPs/NC-900),but also demonstrates high stability and methanol ***,the Cu_(1)/NC-900 based Zn-air battery exhibits higher power density,rechargeability and cyclic stability than the one based on Pt/*** experimental and theoretical investigations demonstrated that the excellent performance of the as-obtained Cu_(1)/NC-900 could be attributed to the synergistic effect between copper coordinated by three N atoms active sites and the neighbouring carbon defect,resulting in elevated Cu d-band centers of Cu atoms and facilitating intermediate desorption for ORR *** study may lead towards the development of highly efficient non-noble metal catalysts for applications in electrochemical energy conversion.

关键词： single atomic sites catalysts nitrogen-doped carbon materials oxygen reduction reaction carbon defect non-noble metal

The Influence of Alkaline Earth Elements on Electronic Properties ofα-Si3N4 via DFT Calculation

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Journal of Wuhan University of technology(materials Science) 2020年第5期35卷 863-871页

作者： ZHANG Jianwen HUANG Zhifeng YIN Ziqian LI Meijuan CHEN Fei SHEN Qiang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan430070China School of Chemistry Chemical Engineering and Life SciencesWuhan University of TechnologyWuhan430070China

We used density functional theory(DFT)calculations to study the influence of alkali earth metal element(AE)doping on the crystal structure and electronic band structure ofα-*** diversity of atomic radii of alkaline earth metal elements results in structural expansion when they were doped into theα-Si3N4 *** energies of the doped structures indicate that dopants prefer to occupy the interstitial site under the nitrogen-deficient environment,while substitute Si under the nitrogen-rich environment,which provides a guide to synthesizingα-Si3N4 with different doping types by controlling nitrogen *** electronic structures,energy levels of the dopants appear in the bottom of the conduction band or the top of the valence band or the forbidden band,which reduces the bandgap ofα-Si3N4.

关键词： first-principles density functional theory calculations alkaline earth elements dopedα-Si3N4 photoluminescence material crystal structure electronic structure