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Highly active macrocyclic nickel(II) complex for hydrogen evolution reaction in neutral aqueous conditions

International Journal of Hydrogen Energy 2023年第87期48卷 33927-33936页

作者： Shahadat, Hossain M. Ahmad, Nazir Khattak, Zafar A.K. Abdur, Rahaman M. Al-Hajri, Rashid Al-Abri, Mohammed Kao, Chih-Ming Younus, Hussein A. Verpoort, Francis State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China Department of Chemistry Faculty of Science Comilla University Comilla3506 Bangladesh Nanotechnology Research Centre Sultan Qaboos University PO Box 17 Al-Khoud PC 123 Oman Department of Chemical and Petroleum Engineering College of Engineering Sultan Qaboos University P.O Box 33 Al Khould Muscat PC 123 Oman Chemistry Department Faculty of Science Fayoum University Fayoum63514 Egypt Department of Chemistry Government College University Lahore Lahore54000 Pakistan Department of Chemistry Faculty of Science Mawlana Bhashani Science and Technology University Tangail1902 Bangladesh National Research Tomsk Polytechnic University Lenin Avenue 30 Tomsk634050 Russia Institute of Environmental Engineering National Sun Yat-Sen University Kaohsiung Taiwan

Hydrogen (H2) production via water splitting under completely aqueous conditions particularly using an earth-abundant component for both half reactions is very appealing and may reduce our dependence on fossil fuels. In this work, we present a water-soluble molecular nickel(II) complex bearing a macrocyclic N‒heterocyclic carbene (NHC)/pyridine hybrid ligand, ([NiL](PF6)2 (L = bis(2‒pyridyl-methylimidazolylidene)methane as a catalyst for hydrogen evolution reaction (HER) under completely aqueous conditions. The catalyst displayed an outstanding catalytic activity for HER in a phosphate electrolyte of neutral pH, as established by a series of techniques. Long-term (11 h) bulk electrolysis at 0.88 V overpotential provides a maximum of 173.5C charge and total ca. 165.08 μmol (∼15 μmol per hour) H2 with Faradaic efficiency of 98%, while without a catalyst less than 3C was produced within the same time. To the best of our knowledge, the investigation of water reduction with Ni–NHC type catalyst under aqueous conditions has not been reported to date. © 2023 Hydrogen Energy Publications LLC

关键词： Catalyst activity

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Intercalation Engineering of Nickle-Cobalt-Layered Double Hydroxide for Long-Lifespan Supercapacitor

SSRN

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SSRN 2023年

作者： Hu, Wenxuan Chen, Lu Geng, Biao Song, Yihu Wu, Ziliang Zheng, Qiang Shan, Gurong Du, Miao MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou310058 China Zhejiang Provincial Key Lab for Chemical and Biological Processing Technology of Farm Product School of Biological and Chemical Engineering Zhejiang University of Science and Technology Hangzhou310023 China State Key Laboratory of Chemical Engineering College of Chemical and Biological Engineering Zhejiang University Hangzhou310058 China Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering Taiyuan030000 China

Layered double hydroxides (LDHs), a class of 2D lamellar intercalating materials, is a promising candidate for high-performance supercapacitors, while its poor cycling stability has always been its Achille’s heel. Although doping metal ions into the host layer is proved to be an effective way to improve the weakness, the effects of intercalated anions on cycling performance have been rarely studied and highly underestimated. In this paper, we prepared a group of NiCo-LDHs with different intercalated anions, including NO3-, Cl-, SO42-, MoO42- and WO42-, which expand the interlayer spacing from 0.73 to 1.07 nm. Interestingly, although expanding the interlayer spacing could increase the specific capacity by providing more electrochemical active sites, it could not guarantee the improvement in cycling performance and rate capability. The correlation between interlayer spacing and cycling performance exhibits a "volcano" plot. The MoO42- intercalated NiCo-LDH with a 0.96 nm interlayer spacing delivers a high specific capacity of 795 C g-1 and the best cycling stability with 80% capacity retention after 20000 cycles, which is better than NiCo-LDH-NO3 (0.73 nm, 50% after 3000 cycles) and NiCo-LDH-WO4 (1.07 nm, 64% after 20000 cycles). By combining the results with the DFT method, the effects of intercalated anion on cycling performance are illustrated. In addition, the asymmetric supercapacitor also exhibits an excellent cycling stability with ~100% capacity retention after 10000 cycles. This study provides new insight to the compositional design of LDH-based electrodes for long-lifespan supercapacitors. © 2023, The Authors. All rights reserved.

关键词： Cobalt compounds

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Enhanced photocatalytic H_(2) production performance of CdS hollow spheres using C and Pt as bi-cocatalysts

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Chinese Journal of Catalysis 2021年第5期42卷 743-752页

作者： Shipeng Tang Yang Xia Jiajie Fan Bei Cheng Jiaguo Yu Wingkei Ho State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina Department of Science and Environmental Studies The Education University of Hong KongTai PoN.T.Hong Kong 999077China

Photocatalytic H2 production from water splitting is an effective method to solve energy crisis and environmental pollution ***,carbon@CdS composite hollow spheres(C@CdS-HS)are fabricated via a facile hydrothermal method using porous carbon hollow spheres(C-HS)as the *** C@CdS-HS shows an excellent photocatalytic H2-generation rate of 20.9 mmol h^(−1) g^(−1)(apparent quantum efficiency of 15.3%at 420 nm),with 1.0 wt%Pt as a cocatalyst under simulated sunlight irradiation;this rate is 69.7,13.9,and 3.9 times higher than that obtained with pure CdS hollow spheres(CdS-HS),C@CdS-HS,and CdS-HS/Pt,*** enhanced photocatalytic H_(2)-evolution activity of C@CdS-HS/Pt is due to the synergistic effect of C and Pt as the *** C-HS serves not only as an active site provider but also as an electron transporter and ***,C-HS has a strong photothermal effect that is induced by near infrared light,which kinetically accelerates the H_(2)-production ***,the underlying charge transfer pathway and process from CdS to C−HS is *** work highlights the potential application of C-HS-based nanocomposites in solar-to-chemical energy conversion.

关键词： CdS hollow sphere Carbon Platinum Bi-cocatalyst Synergistic effect Photocatalytic hydrogen production

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Macroscopic synthesis of ultrafine N–doped carbon nanofibers for superior capacitive energy storage

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Science Bulletin 2019年第21期64卷 1617-1624页

作者： Qiang Yu Jianshuai Lv Zhenhui Liu Ming Xu Wei Yang Kwadwo Asare Owusu Liqiang Mai Dongyuan Zhao Liang Zhou State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China International School of Materials Saence and Engineering Wuhan University of TechnologyWuhan 430070China

Carbon nanofibers(CNFs)with excellent electric conductivity and high surface area have attracted immense research interests in ***,the macroscopic production of CNFs still remains a great ***,ultrafine N–doped CNFs(N–CNFs)with a diameter of$20 nm are synthesized through a simple and scalable sol-gel method based on the self-assembly of phenolic resin and cetyltrimethylammonium *** employed in aqueous supercapacitors,the obtained activated N–CNFs manifest a high gravimetric/areal capacitance(380 Fg-1/1.7 Fcm-2)as well as outstanding rate capability and cycling ***,the activated N–CNFs also demonstrate excellent capacitive performance(330 Fg-1)in flexible quasi-solid-state *** remarkable electrochemical performance as well as the easy and scalable synthesis makes the N–CNFs a highly promising electrode material for supercapacitors.

关键词： Macroscopic synthesis Carbon Nanofibers N–doping Supercapacitor

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A novel bifunctional oxygen electrode architecture enabled by heterostructures self-scaffolding for lithium–oxygen batteries

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Journal of Energy Chemistry 2020年第12期29卷 216-221页

作者： Liang Xiao Zhong Qin Jingyu Yi Haoyang Dong Jinping Liu School of Chemistry Chemical Engineering and Life ScienceWuhan University of Technology.Wuhan 430070HubeiChina State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070HubeiChina State Center for International Cooperation on Designer Low-Carbon&Environmental Materials and School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina

In recent years, as one of the most promising chemical power sources for future society, lithium–oxygen (Li–O2) battery receives great attention due to its extremely high theoretical energy density of 3505 Wh kg^(–1)[1–4]. In practice, large polarization and consequent low energy efficiency currently still hinder the application of Li–O2batteries, which mainly results from the sluggish electrochemical reaction kinetics of oxygen diffusion electrodes in aprotic electrolytes [5]. On one hand, oxygen reduction reaction (ORR)in aprotic electrolytes is intrinsically sluggish due to the difficult charge transfer, the low solubility of oxygen.

关键词： Heterostructure Nanoarray architecture Bifunctional catalysis Oxygen diffusion electrode Lithium–oxygen batteries

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Biomimetic multi-layered protective materials with prestress and a periodic laminated structure

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Journal of Materiomics 2025年

作者： Xin Liu Fan Zhang Ji Zou Weimin Wang Wei Ji Zhengyi Fu Hubei Longzhong Laboratory Wuhan University of Technology Xiangyang Demonstration Zone Xiangyang 441138 Hubei China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China

The nacreous layer of shells has become an excellent biomimetic template of materials due to its unique structure. Inspired by the highly complex multilayered structure of shells, biomimetic layered composite protective materials with outstanding strength, toughness, and impact resistance have been developed. As the hard phase in biomimetic pearlescent layered protective materials, ceramics suffer from inherent low toughness. Applying prestress proved to be an efficient method to enhance their toughness and impact resistance. In this study, prestressed biomimetic periodic laminated (TiB 2 –TiB)/Ti protective materials were fabricated with spark plasma sintering (SPS) technology under the conditions of 1450 °C and 30 MPa in an argon atmosphere. Moreover, both experimental and numerical simulation analyses were conducted to investigate their protective performance. Compared to non-prestressed protective materials, the prestressed constrained materials exhibited the significantly improved protective performance with reduced penetration depth, substantially lower residual velocity, and kinetic energy after impact. This study provided valuable insights into the structural design and performance optimization of other protective materials.

关键词： (TiB 2 -TiB)/Ti Bionic Pre-stress Protective performance Simulation modeling

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Protecting-group-free enantioselective tandem allylic substitution of o-phenylenediamines and o-aminophenols

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Green synthesis and Catalysis 2022年第2期3卷 185-189页

作者： Xuehua Kang Chao Qian He Yang Jicheng Shi Jerome Claverie Wenjun Tang School of Physical Science and Technology Shanghai Tech UniversityShanghai 200031China State Key Laboratory of Bio-Organic and Natural Products Chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China College of Chemistry Maoming Technology Center of Organic MaterialsGuangdong University of Petrochemical TechnologyMaoming 525000China School of Chemistry and Material Sciences Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China Department of Chemistry University of SherbrookeSherbrooke J1K2R1Canada

A protecting-group-free enantioselective tandem allylic substitution of o-phenylenediamines and o-aminophenols is realized for the first time with a Pd-WingPhos catalyst,providing expedient access to a series of chiral vinylsubstituted heterocycles in excellent ee and yields under mild reaction *** protocol is applied successfully to the synthesis of a cholesteryl ester transfer protein(CETP)inhibitor.

关键词： Tandem allylic substitution WingPhos Protecting-group-free Palladium catalysis Enantioselectivity

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Green N1 Additive Modified Perovskite Precursor Enables Effective Manufacturing of Large-Area Solar Cell Modules with High Efficiency and Stability

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SSRN 2023年

作者： Zang, Yue Shao, Tianxiang Jiao, Chuanjia Zhou, Peng Li, Wangnan Cheng, Jiahao Yang, Gaoyuan Tu, Yibo Ye, Jingchuan Li, Guodong Chu, Liang Lu, Shaojian Liang, Guijie Liang, Ying Wang, Jingyang Zhong, Zhicheng Hu, Run Yan, Wensheng Institute of Carbon Neutrality and New Energy School of Electronics and Information Hangzhou Dianzi University Hangzhou310018 China Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices Hubei University of Arts and Science Xiangyang441053 China Hubei Longzhong laboratory Xiangyang441000 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan430070 China Hubei Institute of Aerospace Chemotechnology Xiangyang441003 China School of Energy and Power Engineering Huazhong University of Science and Technology Wuhan430074 China

Perovskite solar cells (PSCs) have been continuously breaking the solar photoelectric power conversion efficiency (PCE) record, while two long-standing challenges remain formidable on the practical commercialization path of PSCs, i.e. effective large-area manufacturing and high device operational stability. Here, we report a green additive of N-methyl-2-piperidone (N1) to modify the perovskite precursor, enabling the one-step mass manufacturing of high-quality large-area perovskite films with enhanced PCE and operational stability. The results show that due to the stronger complexation ability of N1 additive with PbI2, the generated PbI2-N1 complex can effectively prevent the preferential nucleation and realize lead halide-framework template-assistant crystallization reaction with organic cation in the one-step solution preparation of perovskite (FAPbI3)0.95(MAPbBr3)0.05 thin films, which result in the uniform grain size and smooth, dense film quality. Therefore, the PSCs device with small active area of 0.09 cm2 exhibits an efficiency of 22.2%, which is further improved to 23.2% by passivating the perovskite interface using PEAI. Moreover, highly-efficient slot-die printed 5×5 cm2 PSC module has been obtained with a champion PCE of 21% and improved operational stability over 1000 h. This work demonstrated a new strategy to realize high-quality large-scale perovskite films for solution-processed PSC modules, and may be further improved and extended to other kinds of PSCs and perovskite light-emitting diodes and detectors. © 2023, The Authors. All rights reserved.

关键词： Nucleation

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Emerging heterostructured C3N4 photocatalysts for photocatalytic environmental pollutant elimination and sterilization

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Inorganic Chemistry Frontiers 2023年第13期10卷 3756-3780页

作者： Yang Ding Chunhua Wang Lang Pei Soumyajit Maitra Qinan Mao Runtian Zheng Meijiao Liu Yun Hau Ng Jiasong Zhong Li-Hua Chen Bao-Lian Su Center of Advanced Optoelectronic Materials College of Materials and Environmental Engineering Hangzhou Dianzi University Hangzhou 310018 China School of Energy and Environment City University of Hong Kong Tat Chee Avenue Kowloon Hong Kong China Department of Materials University of Oxford Oxford UK Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles Namur Belgium Department of Chemistry Zhejiang Sci-Tech University Hangzhou 310018 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road 430070 Wuhan Hubei China

Photocatalysis is deemed a highly prominent technology to solve environmental problems such as pollution, CO2 emission and bacterial contamination. As an important photocatalyst, g-C3N4 has attracted a great amount of...

Photocatalysis is deemed a highly prominent technology to solve environmental problems such as pollution, CO₂ emission and bacterial contamination. As an important photocatalyst, g-C3N4 has attracted a great amount of attention in environmental remediation owing to its good stability, excellent light response, low cost and environmentally friendly properties. However, the pristine g-C3N4 photocatalyst generally suffers from serious photoinduced charge carrier recombination, poor surface active sites, and insufficient visible light harvesting, thereby leading to unsatisfactory photocatalytic performance. Heterostructured C₃N₄ photocatalysts have recently become a research focus in environmental fields thanks to their fast photoexcited electron–hole pair dissociation, broadened visible light response range, and sufficient photoredox capability. Herein, we critically review the up-to-date developments of heterostructured C₃N₄ photocatalysts in organic pollutant elimination, heavy metal ion reduction, CO₂ conversion and bacterial inactivation. Meanwhile, the strategies for constructing efficient C₃N₄ based heterostructures with enhanced environmental photocatalytic capability are thoroughly described, which should help readers to quickly acquire in-depth knowledge and to inspire new concepts in heterostructure engineering. Finally, the challenges and opportunities in fabricating heterostructured C₃N₄ photocatalysts for large-scale and commercial applications are discussed to give a clear study direction in this field.

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Weaving 3D highly conductive hierarchically interconnected nanoporous web by threading MOF crystals onto multi walled carbon nanotubes for high performance Li-Se battery

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能源化学 2021年第8期59卷 396-404页

作者： Chao Li Yingying Wang Hongyan Li Jing Liu Jianping Song Luca Fusaro Zhi-Yi Hu Yanxin Chen Yu Li Bao-Lian Su Laboratory of Inorganic Materials Chemistry (CMI) University of Namur B-5000 Namur Belgium Namur Institute of Structured Matter (NISM) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Institute of Microscale Optoelectronics College of Physics and Optoelectronic Engineering Collaborative Innovation Centre for Optoelectronic Science & Technology Shenzhen University Shenzhen 518060 Guangdong China Laboratory of Inorganic Materials Chemistry (CMI) University of Namur B-5000 Namur Belgium Namur Institute of Structured Matter (NISM) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Laboratory of Living Materials at the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China Namur Institute of Structured Matter (NISM) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Laboratory of Inorganic Materials Chemistry (CMI) University of Namur B-5000 Namur Belgium Namur Institute of Structured Matter (NISM) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Laboratory of Living Materials at the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei China

Lithium-selenium (Li-Se) battery has attracted growing ***,its practical application is still impeded by the shuttle effect of the formed ***,we report in-situ hydrothermal weaving the three-dimensional (3D) highly conductive hierarchically interconnected nanoporous web by threading microporous metal organic framework MIL-68(Al) crystals onto multi-walled carbon nanotubes (MWCNTs).Such 3D hierarchically nanoporous web (3D MIL-68 (Al)@MWCNTs web) with a very high surface area,a large amount of micropores,electrical conductivity and elasticity strongly traps the soluble polyselenides during the electrochemical reaction and significantly facilitates lithium ion diffusion and electron *** dynamic calculation confirmed the strong affinity of MIL-68 (Al) for the adsorption of polyselenides,quite suitable for Li-Se *** hexahedral channels (1.56 nm) are more efficient for the confinement of polyselenides and for the diffusion of electrolytes compared to their smaller triangular channels (0.63 nm).All these excellent characteristics of 3D MIL-68 (Al)@MWCNTs web with suitable confinement of a large amount of selenium and the conductive linkage between MIL-68(Al) host by MWCNTs result in a high capacity of 453 mAh/g at 0.2C with 99.5％ coulombic efficiency after 200 cycles with significantly improved cycle stability and rate *** 3D MIL-68 (Al)@MWCNTs web presents a good performance in Li-Se battery in term of the specific capacity and cycling stability and also in terms of rate performance compared with all the metal-organic framework (MOF) based or MOF derived porous carbons used in Li-Se battery.

关键词： Lithium selenium battery Selenium confinement 3D hierarchically nanoporous web Metal–organic framework (MOF) Multi walled carbon nanotubes

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