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Decade Milestone Advancement of Defect-Engineered g-C_(3)N_(4) for Solar Catalytic Applications

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Nano-Micro Letters 2024年第4期16卷 153-218页

作者： Shaoqi Hou Xiaochun Gao Xingyue Lv Yilin Zhao Xitao Yin Ying Liu Juan Fang Xingxing Yu Xiaoguang ma tianyi ma Dawei Su School of mathematical and Physical Sciences Faculty of ScienceUniversity of Technology Sydney(UTS)SydneyNSW 2007Australia Laboratory of Plasma and Energy Conversion School of Physics and Optoelectronic EngineeringLudong University186 Middle Hongqi RoadYantai 264025People’s Republic of China School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083People’s Republic of China Department of Chemistry The University of Tokyo7‑3‑1 HogoBunkyoTokyoJapan School of Science STEM CollegeRMIT UniversityMelbourneVIC 3000Australia

Over the past decade, graphitic carbon nitride(g-C_(3)N_(4)) has emerged as a universal photocatalyst toward various sustainable carbo-neutral technologies. Despite solar applications discrepancy, g-C_(3)N_(4) is still confronted with a general fatal issue of insufficient supply of thermodynamically active photocarriers due to its inferior solar harvesting ability and sluggish charge transfer dynamics. Fortunately, this could be significantly alleviated by the “all-in-one” defect engineering strategy, which enables a simultaneous amelioration of both textural uniqueness and intrinsic electronic band structures. To this end, we have summarized an unprecedently comprehensive discussion on defect controls including the vacancy/non-metallic dopant creation with optimized electronic band structure and electronic density, metallic doping with ultraactive coordinated environment(M–N_(x), M–C_(2)N_(2), M–O bonding), functional group grafting with optimized band structure, and promoted crystallinity with extended conjugation π system with weakened interlayered van der Waals interaction. Among them, the defect states induced by various defect types such as N vacancy, P/S/halogen dopants, and cyano group in boosting solar harvesting and accelerating photocarrier transfer have also been emphasized. More importantly, the shallow defect traps identified by femtosecond transient absorption spectra(fs-TAS) have also been highlighted. It is believed that this review would pave the way for future readers with a unique insight into a more precise defective g-C_(3)N_(4) “customization”, motivating more profound thinking and flourishing research outputs on g-C_(3)N_(4)-based photocatalysis.

关键词： Defect engineering g-C_(3)N_(4) Electronic band structures Photocarrier transfer kinetics Defect states

Deep learning-based semantic segmentation of human features in bath scrubbing robots

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Biomimetic Intelligence & Robotics 2024年第1期4卷 70-79页

作者： Chao Zhuang tianyi ma Bokai Xuan Cheng Chang Baichuan An Minghuan Yin Hao Sun School of Artificial Intelligence and Data Science Hebei University of TechnologyTianjin 300401China Engineering Research Center of Intelligent Rehabilitation Device and Detection Technology Ministry of EducationTianjin 300401China

With the rise in the aging population,an increase in the number of semidisabled elderly individuals has been noted,leading to notable challenges in medical and healthcare,exacerbated by a shortage of nursing staff.This study aims to enhance the human feature recognition capabilities of bath scrubbing robots operating in a water fog environment.The investigation focuses on semantic segmentation of human features using deep learning methodologies.Initially,3D point cloud data of human bodies with varying sizes are gathered through light detection and ranging to establish human models.Subsequently,a hybrid filtering algorithm was employed to address the impact of the water fog environment on the modeling and extraction of human regions.Finally,the network is refined by integrating the spatial feature extraction module and the channel attention module based on PointNet.The results indicate that the algorithm adeptly identifies feature information for 3D human models of diverse body sizes,achieving an overall accuracy of 95.7%.This represents a 4.5%improvement compared with the PointNet network and a 2.5%enhancement over mean intersection over union.In conclusion,this study substantially augments the human feature segmentation capabilities,facilitating effective collaboration with bath scrubbing robots for caregiving tasks,thereby possessing significant engineering application value.

关键词： 3D point cloud Human model LiDAR Semantic segmentation

Enhancing Green Ammonia Electrosynthesis Through Tuning Sn Vacancies in Sn‑Based MXene/ maX Hybrids

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Nano-Micro Letters 2024年第5期16卷 154-168页

作者： Xinyu Dai Zhen‑Yi Du Ying Sun Ping Chen Xiaoguang Duan Junjun Zhang Hui Li Yang Fu Baohua Jia Lei Zhang Wenhui Fang Jieshan Qiu tianyi ma Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced materials of Liaoning Province College of ChemistryInstitute of Clean Energy ChemistryLiaoning UniversityShenyang 110036People’s Republic of China State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024People’s Republic of China School of Chemistry and Chemical Engineering Anhui UniversityHefei 230601People’s Republic of China School of Chemical Engineering The University of AdelaideAdelaideSA 5005Australia State Key Laboratory of High‑Efficiency Utilization of Coal and Green Chemical Engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021NingxiaPeople’s Republic of China School of Science RMIT UniversityMelbourneVIC 3000Australia Guangdong Provincial Key Laboratory of Advanced Energy Storage materials School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640People’s Republic of China College of Chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia production.However,relevant out-lab research is still in its infancy.Herein,a novel Sn-based MXene/maX hybrid with abundant Sn vacancies,Sn@Ti_(2)CTX/Ti_(2)SnC–V,was synthesized by controlled etching Sn@Ti_(2)SnC maX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N2 reduction.Due to the synergistic effect of MXene/maX heterostructure,the existence of Sn vacancies and the highly dispersed Sn active sites,the obtained Sn@Ti2CTX/Ti_(2)SnC–V exhibits an optimal NH_(3) yield of 28.4μg h^(−1) mg_(cat)^(−1) with an excellent FE of 15.57% at−0.4 V versus reversible hydrogen electrode in 0.1 M Na_(2)SO_(4),as well as an ultra-long durability.Noticeably,this catalyst represents a satisfactory NH3 yield rate of 10.53μg h^(−1) mg^(−1) in the home-made simulation device,where commercial electrochemical photovoltaic cell was employed as power source,air and ultrapure water as feed stock.The as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic analysis.This work is of significance for large-scale green ammonia production.

关键词： Green ammonia synthesis N2 electroreduction Renewable energy Sn MXene/maX hybrid

Near-infrared non-fused electron acceptors for efficient organic photovoltaics

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Chinese Chemical Letters 2024年第4期35卷 436-441页

作者： Wenxiang ma Xinyu He tianyi Chen De-Li ma Hongzheng Chen Chang-Zhi Li State Key Laboratory of Silicon and Advanced Semiconductor materials Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China

Developing narrow-bandgap organic semiconductors is important to facilitate the advancement of organic photovoltaics(OPVs). Herein, two near-infrared non-fused ring acceptors(NIR NFRAs), PTBFTT-F and PTBFTT-Cl have been developed with A-π_A-π_D-D-π_D-π_A-A non-fused structures. It is revealed that the introduction of electron deficient π-bridge(π_A) and multiple intramolecular noncovalent interactions effectively retained the structural planarity and intramolecular charge transfer of NFRAs, extending strong NIR photon absorption up to 950 nm. Further, the chlorinated acceptor, with the enlarged π-surface compared to the fluorinated counterpart, promoted not only molecular stacking in solid, but also the desirable photochemical stability in ambient, which are helpful to thereby improve the exciton and charge dynamics for the corresponding OPVs. Overall, this work provides valuable insights into the design of NIR organic semiconductors.

关键词： Organic photovoltaic Near-infrared Non-fused electron acceptor Noncovalent interaction Stability

Effect of Cryogenic Treatment on Microstructure and Tribological Property Evolution of Electron Beam Melted Ti6Al4V

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Journal of Wuhan University of Technology(materials Science) 2024年第4期39卷 1010-1017页

作者：黄西娜 ma Xiaowen XU tianyi School of Mechanical and Electrical Engineering China University of Mining and Technology-BeijingBeijing 100083China School of Engineering and Technology China University of GeosciencesBeijing 100083China

Cryogenic treatment was used to improve the tribological properties of Ti6Al4V artificial hip joint implants.Cryogenic treatment at-196℃with different holding time were carried out on Ti6Al4V specimens fabricated using electron beam melting(EBM),and their microstructure and tribological properties evolution were systematically analyzed by scanning electron microscopy(SEM),vickers hardness,and wear tests.The experimental results show that the as-fabricated specimen consists of lamellarαphase andβcolumnar crystal.While,the thickness of lamellarαphase decreased after cryogenic treatment.In addition,it can be found that the fineαphase was precipitated and dispersed between the lamellarαphase with the holding time increase.Vickers hardness shows a trend of first increasing and then decreasing.The wear rate of the specimen cryogenic treated for 24 h is the minimum and the average friction coefficient is 0.50,which is reduced by 14.61%compared with the as-fabricated.The wear mechanism of the as-fabricated specimen is severe exfoliation,adhesive,abrasive,and slight fatigue wear.However,the specimen cryogenic treated for 24 h shows slight adhesive and abrasive wear.It can be concluded that it is feasibility of utilizing cryogenic treatment to reduce the wear of EBMed Ti6Al4V.

关键词： electron beam melting(EBM) cryogenic treatment microstructure vickers hardness tribological property

Gradient solid electrolyte interphase induced by bisfuoroacetamide for stable lithium metal batteries

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Journal of Energy Chemistry 2022年第3期31卷 676-679,I0018页

作者： Qin Zhao tianyi ma Institute of Clean Energy Chemistry Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning ProvinceCollege of ChemistryLiaoning UniversityShenyang 110036LiaoningChina Centre for Translational Atomaterials Swinburne University of TechnologyHawthornVIC 3122Australia

With continuous development of portable electronics and electric vehicles,the conventional lithium-ion batteries(LIBs)could not meet the demand for higher energy density[1,2].Instead,the lithium metal batteries(LMBs)are regarded as the most promising candidate for next generation energy storage systems due to the highest specific capacity(3860 mah g^(-1))and lowest redox potential(-3.04 V vs.standard hydrogen electrode)of Li metal[3,4].

关键词： Bisfuoroacetamide Lithium metal batteries Electrolyte interphase

Dual‑Doped Nickel Sulfide for Electro‑Upgrading Polyethylene Terephthalate into Valuable Chemicals and Hydrogen Fuel

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纳微快报:英文版 2023年第11期15卷 385-399页

作者： Zhijie Chen Renji Zheng Teng Bao tianyi ma Wei Wei Yansong Shen Bing‑Jie Ni Centre for Technology in Water and Wastewater School of Civil and Environmental EngineeringUniversity of Technology SydneySydneyNSW 2007Australia School of Minerals Processing and Bioengineering Central South UniversityChangsha 410083People’s Republic of China School of Biology Food and Environment EngineeringHefei UniversityHefei 230601People’s Republic of China School of Science STEM CollegeRMIT UniversityMelbourneVIC 3000Australia School of Chemical Engineering University of New South WalesSydneyNSW 2052Australia

Electro-upcycling of plastic waste into value-added chemicals/fuels is an attractive and sustainable way for plastic waste management.Recently,electrocatalytically converting polyethylene terephthalate(PET)into formate and hydrogen has aroused great interest,while developing low-cost catalysts with high efficiency and selectivity for the central ethylene glycol(PET monomer)oxidation reaction(EGOR)remains a challenge.Herein,a high-performance nickel sulfide catalyst for plastic waste electro-upcycling is designed by a cobalt and chloride co-doping strategy.Benefiting from the interconnected ultrathin nanosheet architecture,dual dopants induced upshifting d band centre and facilitated in situ structural reconstruction,the Co and Cl co-doped Ni_(3)S_(2)(Co,Cl-NiS)outperforms the singledoped and undoped analogues for EGOR.The self-evolved sulfide@oxyhydroxide heterostructure catalyzes EG-to-formate conversion with high Faradic efficiency(>92%)and selectivity(>91%)at high current densities(>400 ma cm^(−2)).Besides producing formate,the bifunctional Co,Cl-NiS-assisted PET hydrolysate electrolyzer can achieve a high hydrogen production rate of 50.26 mmol h^(−1)in 2 M KOH,at 1.7 V.This study not only demonstrates a dual-doping strategy to engineer cost-effective bifunctional catalysts for electrochemical conversion processes,but also provides a green and sustainable way for plastic waste upcycling and simultaneous energy-saving hydrogen production.

关键词： Hydrogen energy Electro-upcycling Structural reconstruction Organic waste upcycling d Band centre

Redox-etching induced porous carbon cloth with pseudocapacitive oxygenic groups for flexible symmetric supercapacitor

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Journal of Energy Chemistry 2022年第1期31卷 136-143,I0005页

作者： Xu Han Zi-Hang Huang Fanjin Meng Baohua Jia tianyi ma Institute of Clean Energy Chemistry Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning ProvinceCollege of ChemistryLiaoning UniversityShenyang 110036LiaoningChina Centre for Translational Atomaterials School of ScienceSwinburne University of TechnologyHawthornVIC 3122Australia

Constructing high-performance electrodes with both wide potential window(e.g.≥2 V in aqueous electrolyte)and excellent mechanical flexibility represents a great challenge for supercapacitors.Because of the outstanding conductivity and flexibility,carb on cloth(CC)has show n unlimited prospects for constructing flexible electrodes,but is rarely used directly as electrode material due to its electrochemical inertness and small specific surface area.To tackle these two critical limitations,we design a novel redox-etching strategy to synthesize CC-based electrode with 3D interconnecting pore structure.The sponge-like highly porous CC was further activated by strong oxidant to form abundant oxygenic groups,which occupy the interior and surface of current collector to render substantial pseudocapacitance.The as-synthesized CC electrode yielded an impressive capacitance of 4035 mF cm^(-2) at 3 ma cm^(-2) and satisfying cycling durability in a wide potential range of-1-1 V vs.SCE,which surpass the majority of reported CC-based electrodes.A symmetric supercapacitor with stable voltage of 2 V is assembled and delivers remarkable energy density of 6.57 mWh cm^(-3).Significantly,the device demonstrates an unparalleled flexibility with no capacitive decay after 100 bending cycles.This facile chemical etching and post-treatment processes are designed for large-scale manufacturing of the CC electrodes by providing high surface area and abundant electrochemically active sites,promising for industry application.The innovative synthetic strategy ope ns up new opportunities for high-performance flexible en ergy storage.

关键词： Porous carbon fiber Hierarchical pores Oxygenic groups Wide potential window High-performance supercapacitors

Metal-Free 2D/2D van der Waals Heterojunction Based on Covalent Organic Frameworks for Highly Efficient Solar Energy Catalysis

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Nano-Micro Letters 2023年第9期15卷 15-30页

作者： Ge Yan Xiaodong Sun Yu Zhang Hui Li Hongwei Huang Baohua Jia Dawei Su tianyi ma Institute of Clean Energy Chemistry Key Laboratory for Green Synthesis and Preparative Chemistry of Adv.Mater.College of ChemistryLiaoning UniversityShenyang 110036People’s Republic of China School of Science RMIT UniversityMelbourneVIC 3000Australia Faculty of Science School of Mathematical and Physical SciencesUniversity of Technology SydneySydneyNSW 2007Australia Beijing Key Laboratory of materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral MaterialsSchool of Materials Science and TechnologyChina University of GeosciencesBeijing 100083People’s Republic of China

Covalent organic frameworks(COFs)have emerged as a kind of rising star materials in photocatalysis.However,their photocatalytic activities are restricted by the high photogenerated electron-hole pairs recombination rate.Herein,a novel metal-free 2D/2D van der Waals heterojunction,composed of a two-dimensional(2D)COF with ketoenamine linkage(TpPa-1-COF)and 2D defective hexagonal boron nitride(h-BN),is successfully constructed through in situ solvothermal method.Benefitting from the presence of VDW heterojunction,larger contact area and intimate electronic coupling can be formed between the interface of TpPa-1-COF and defective h-BN,which make contributions to promoting charge car-riers separation.The introduced defects can also endow the h-BN with porous structure,thus providing more reactive sites.Moreover,the TpPa-1-COF will undergo a structural transformation after being integrated with defective h-BN,which can enlarge the gap between the conduction band position of the h-BN and TpPa-1-COF,and suppress electron backflow,corroborated by experimental and density functional theory calculations results.Accordingly,the resulting porous h-BN/TpPa-1-COF metal-free VDW heterojunction displays out-standing solar energy catalytic activity for water splitting without co-catalysts,and the H_(2) evolution rate can reach up to 3.15 mmol g^(−1) h^(−1),which is about 67 times greater than that of pristine TpPa-1-COF,also surpassing that of state-of-the-art metal-free-based photocatalysts reported to date.In particular,it is the first work for constructing COFs-based heterojunctions with the help of h-BN,which may provide new avenue for designing highly efficient metal-free-based photocatalysts for H_(2) evolution.

关键词： Covalent organic frameworks 2D/2D van der Waals heterojunction Metal-free photocatalyst