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Construction of N-doped carbon frames anchored with Co single atoms and Co nanoparticles as robust electrocatalyst for hydrogen evolution in the entire pH range

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Journal of Energy Chemistry 2022年第4期31卷 147-156页

作者： Minmin Wang Min Li Yilin Zhao Naiyou Shi Hui Zhang Yuxue Zhao Yaru Zhang Haoran Zhang Wenhong Wang Kaian Sun Yuan Pan Shoujie Liu houyu zhu Wenyue Guo Yanpeng Li Yunqi Liu Chenguang Liu State Key Laboratory of Heavy Oil Processing China University of Petroleum(East China)Qingdao 266580ShandongChina School of Materials Science and Engineering China University of Petroleum(East China)Qingdao 266580ShandongChina College of Chemistry and Materials Science Anhui Normal UniversityWuhu 241000AnhuiChina

The development of low-cost, efficient, and high atomic economy electrocatalysts for hydrogen evolution reaction(HER) in the entire p H range for sustainable hydrogen production is of great importance but still challenging. Herein, we synthesize a highly dispersed N-doped carbon frames(NCFs) anchored with Co single atoms(SAs) and Co nanoparticles(NPs) catalyst by a doping-adsorption-pyrolysis strategy for electrocatalytic hydrogen evolution. The Co SAs-Co NPs/NCFs catalyst exhibits an excellent HER activity with small overpotential, low Tafel slope, high turnover frequency as well as remarkable stability. It also exhibits a superior HER performance in the entire p H range. Combining with experimental and theoretical calculation, we find that Co SAs with Co-N_(3) coordination structure and Co NPs have a strong interaction for promoting synergistic HER electrocatalytic process. The H_(2)O molecule is easily activated and dissociated on Co NPs, while the generated H^(*) is easily adsorbed on Co SAs for HER, which makes the Co SAs-Co NPs/NCFs catalyst exhibit more suitable H adsorption strength and more conducive to the activation and dissociation of H_(2)O molecules. This work not only proposes a novel idea for constructing coupling catalyst with atomic-level precision, but also provides strong reference for the development of high-efficiency HER electrocatalysts for practical application.

关键词： Single-atom catalyst Doping-adsorption-pyrolysis strategy Structure regulation Synergistic electrocatalysis EXAFS

Targeted bottom-up synthesis of 1T-phase MoS2 arrays with high electrocatalytic hydrogen evolution activity by simultaneous structure and morphology engineering

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Nano Research 2018年第8期11卷 4368-4379页

作者： Kaian Sun Yunqi Liu Yuan Pan houyu zhu Jinchong Zhao Lingyou Zeng Zhi Liu Chenguang Liu State Key Laboratory of Heavy Oil Processing College of Chemical Engineering China University of Petroleum (East China) 66 WestChangjiang Road Qingdao 266580 China Department of Chemistry Tsinghua University Beijing 100084 China College of Science China University of Petroleum (East China) 66 West Changjiang Road Qingdao 266580 China

The incorporation of small guest molecules or ions by bottom-up hydrothermal synthesis has recently emerged as a promising new way to engineer 1T-phase MoS2 with high hydrogen evolution reaction （HER） activity. However, the mechanism of the associated structural evolution remains elusive and controversial, leading to a lack of effective routes to prepare 1T-phase MoS2 with controlled structure and morphology, along with high purity and stability. Herein, urea is chosen as precursor of small molecules or ions to simultaneously engineer the phase （16.4%, - 69.4%, and -90.2% of 1T phase） and size （98.8, - 151.6, and - 251.8 nm for the 90.2% 1T phase） of MoS2 nanosheets, which represent an ideal model system for investigating the structural evolution in these materials, as well as developing a new type of 1T-phase MoS2 arrays. Using reaction intermediate monitoring and theoretical calculations, we show that the oriented growth of 1T-phase MoS2 is controlled by ammonia-assisted assembly recrystallization, and stabilization processes. A superior HER performance in acidic media is obtained, with an overpotential of only 76 mV required to achieve a stable current density of 10 ***-2 for 15 h. This excellent performance is attributed to the unique array structure, involving well-dispersed, edge-terminated, and high-purity 1T-phase MoS2 nanosheets.

关键词： molybdenum disulfide bottom-up synthesis morphology engineering.structure engineering hydrogen evolution density functional theory

Reaction environment self-modification on low-coordination Ni^(2+)octahedra atomic interface for superior electrocatalytic overall water splitting

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Nano Research 2020年第11期13卷 3068-3074页

作者： Kaian Sun Lei Zhao Lingyou Zeng Shoujie Liu houyu zhu Yanpeng Li Zheng Chen Zewen zhuang Zhaoling Li Zhi Liu Dongwei Cao Jinchong Zhao Yunqi Liu Yuan Pan Chen Chen State Key Laboratory of Heavy Oil Processing College of Chemical EngineeringChina University of Petroleum(East China)Qingdao266580China Department of Chemistry Tsinghua UniversityBeijing100084China College of Science China University of Petroleum(East China)Qingdao266580China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of TextilesDonghua UniversityShanghai201620China

Large scale synthesis of high-efficiency bifunctional electrocatalyst based on cost-effective and earth-abundant transition metal for overall water splitting in the alkaline environment is indispensable for renewable energy *** this regard,meticulous design of active sites and probing their catalytic mechanism on both cathode and anode with different reaction environment at molecular-scale are vitally ***,a coordination environment inheriting strategy is presented for designing low-coordination Ni^(2+)octahedra(L-Ni-8)atomic interface at a high concentration(4.6 at.%).Advanced spectroscopic techniques and theoretical calculations reveal that the self-matching electron delocalization and localization state at L-Ni-8 atomic interface enable an ideal reaction environment at both cathode and *** improve the efficiency of using the self-modification reaction environment at L-Ni-8,all of the structural features,including high atom economy,mass transfer,and electron transfer,are integrated together from atomic-scale to *** high current density of 500 mA/cm2,the samples synthesized at gram-scale can deliver low hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)overpotentials of 262 and 348 mV,respectively.

关键词： atomic interface effect overall water splitting high current density reaction environment self-modification density functional theory

Carbon Emission Effects Driven by Evolution of Chinese Dietary Structure from 1987 to 2020

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Chinese Geographical Science 2024年第1期34卷 181-194页

作者： zhu Yuanyuan ZHANG Yan zhu Xiaohua Key Laboratory of Geographic Process Analysis&Simulation Hubei Province Central China Normal UniversityWuhan430079China Institute of Geographic Sciences and Natural Resources Research Chinese Academy of SciencesBeijing100101China

Exploring carbon emission effects based on the evolution of residents’ dietary structure to achieve the carbon neutrality goal and mitigate climate change is an important *** study took China as the research object(data excluding Hong Kong,Macao and Taiwan) and used the carbon emission coefficient method to quantitatively measure the food carbon emissions from 1987–2020,then analyzed the carbon emission effects under the evolution of dietary *** results showed that during the study period,the Chinese dietary structure gradually changed to a high-carbon consumption *** dietary structure of urban residents developed to a balanced one,while that of rural residents developed to a high-quality *** the study period,the per capita food carbon emissions and total food consumption of Chinese showed an increasing *** per capita food carbon emissions of residents in urban and rural showed an overall upward *** total food carbon emissions in urban increased significantly,while that in rural increased first and then *** influence of beef and mutton on carbon emissions is the highest in dietary *** with the balanced dietary pattern,the food carbon emissions of Chinese residents had not yet reached the peak,but were evolving to a high-carbon consumption pattern.

关键词： dietary structure structural evolution carbon emission effects carbon neutrality China

Synergistic catalysis of the N-hydroxyphthalimide on flower-like bimetallic metal-organic frameworks for boosting oxidative desulfurization

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Petroleum Science 2024年第1期21卷 674-682页

作者： Jing He Kun zhu Wei Jiang Dong-Ao zhu Lin-Hua zhu Hai-Yan Huang Wen-Shuai zhu Hua-Ming Li Institute for Energy Research Jiangsu UniversityZhenjiang212013JiangsuChina College of Chemistry and Chemical Engineering Hainan Normal UniversityKey Laboratory of Water Pollution Treatment and Resource Reuse of Hainan ProvinceHaikou571158HainanChina

Synergic catalytic effect between active sites and supports greatly determines the catalytic activity for the aerobic oxidative desulfurization of fuel *** this work,Ni-doped Co-based bimetallic metal-organic framework(CoNi-MOF)is fabricated to disperse N-hydroxyphthalimide(NHPI),in which the whole catalyst provides plentiful synergic catalytic effect to improve the performance of oxidative desulfurization(ODS).As a bimetallic MOF,the second metal Ni doping results in the flower-like morphology and the modification of electronic properties,which ensure the exposure of NHPI and strengthen the synergistic effect of the overall *** with the monometallic Co-MOF and naked NHPI,the NHPI@CoNi-MOF triggers the efficient activation of molecular oxygen and improves the ODS performance without an *** sulfur removal of dibenzothiophene-based model oil reaches 96.4%over the NHPI@CoNi-MOF catalyst in 8 h of ***,the catalytic product of this aerobic ODS reaction is sulfone,which is adsorbed on the catalyst surface due to the difference in *** work provides new insight and strategy for the design of a strong synergic catalytic effect between NHPI and bimetallic supports toward high-activity aerobic ODS materials.

关键词： Metal-organic frameworks Doped Bimetallic N-hydroxyphthalimide Aerobic processes Oxidative desulfurization

Efficient Removal of Phosphate from Aqueous Solutions Using Corundum-hollow-spheres Supported Caclined Hydrotalcite Porous Thin Films

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Journal of Wuhan University of Technology(Materials Science) 2024年第1期39卷 44-49页

作者：刘云才 zhu Chen School of Architecture and Materials Engineering Hubei Second Normal UniversityWuhan 430205China

Phosphate was removed from aqueous environment by corundum-hollow-spheres supported caclined hydrotalcite (cHT) thin films. Mg-Al-CO3 hydrotalcite (HT) thin films were deposited on corundumhollow-sphere substrates by hydrothermal homogeneous precipitation at 120℃for 30-240 min and cHT thin films were obtained by annealing of the HT thin films at 500℃for 180 min. Their crystal phase, morphology and microstructure were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM).The results show that homogeneous, well-crystallized and hierarchical flower-like thin films were deposited firmly on the surface of the corundum. The mechanism of nucleation and growth of the HT thin films was fitted well with the anion coordination polyhedron growth unit model. To determine the absorption of phosphate by this adsorbent, different bed depth (10-30 cm) and flow rate (1.0-3.0 m L/min) were examined by column experiments. The highest removal efficiency of phosphate amounted to 98.5%under optimum condition (pH=7.2). The adsorption capacity increased as the bed depth increased and decreased as the flow rate increased.

关键词： adsorption phosphate hydrotalcite corundum-hollow-sphere hydrothermal homogeneous precipitation thermal anneal

A review of recent advances in the effects of surface and interface properties on marine propellers

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Friction 2024年第2期12卷 185-214页

作者： Manfu zhu Liran MA State Key Laboratory of Tribology in Advanced Equipment Tsinghua UniversityBeijing 100084China

Marine propellers are important propulsion devices for both surface ships and underwater *** severe environmental problems have required further performance enhancement for ***,traditional methods to improve propeller performances through geometrical and structural optimizations have been extensively investigated,while the underlying mechanisms of the effects of surface and interface properties on marine propellers are still far from being fully *** paper presented a comprehensive review of recent advances in the effects of surface and interface properties,such as surface roughness and surface wettability,on marine propellers with an emphasis on the significant improvements in both hydrodynamic and cavitation performances,hoping to arouse more in-depth investigations in the field of surface/interface science and technologies on marine propellers,and also promote the state-of-the-art technologies,such as superlubricity technology,into practical applications.

关键词： marine propellers hydrodynamics cavitation surface roughness surface wettability

Engineering applications and technical challenges of active array microsystems

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Frontiers of Information Technology & Electronic Engineering 2024年第3期25卷 342-368页

作者： Jiaguo LU Haoran zhu East China Research Institute of Electronic Engineering Hefei 230039China School of Electronic and Information Engineering Anhui UniversityHefei 230601China

In the post-Moore era,the development of active phased array antennas will inevitably trend towards active array *** this paper,the characteristics and composition of the active array antenna are briefly *** to the high efficiency,low profile,and light weight of the active array microsystems,the application prospects and advantages in the engineering of multi-functional airborne radar,spaceborne radar,and communication systems are ***,according to the characteristics of the post-Moore era of integrated circuits,scientific and technological problems in the active array microsystems are presented,including multi-scale,multi-signal,and multi-physics field *** challenges are also discussed,such as new architectures and algorithms,miniaturization of passive components,novel materials and processes,ultra-wideband technology,and new interdisciplinary technological *** paper is expected to inspire in-depth research on active array microsystems.

关键词： Microelectronics Heterogeneous integration Packaging materials Antenna array microsystems Multi-functional radar Communication

Leaching kinetics of fluorine during the aluminum removal from spent Li-ion battery cathode materials

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Journal of Environmental Sciences 2024年第4期138卷 312-325页

作者： Shengjie Li Jianxin zhu Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China

The high content of aluminum(Al)impurity in the recycled cathode powder seriously affects the extraction efficiency of Nickel,Cobalt,Manganese,and Lithium resources and the actual commercial value of recycled materials,so Al removal is crucially important to conform to the industrial standard of spent Li-ion battery cathode *** this work,we systematically investigated the leaching process and optimum conditions associated with Al removal from the cathode powder materials collected in a wet cathode-powder peeling and recycling production line of spent Li-ion batteries(LIBs).Moreover,we specifically studied the leaching of fluorine(F)synergistically happened along with the removal process of Al,which was not concerned about in other studies,but one of the key factors affecting pollution prevention in the recovery *** mechanism of the whole process including the leaching of Al and F from the cathode powder was indicated by using NMR,FTIR,and XPS,and a defluoridation process was preliminarily investigated in this *** leaching kinetics of Al could be successfully described by the shrinking core model,controlled by the diffusion process and the activation energy was 11.14 kJ/***,the leaching of F was attributed to the dissolution of LiPF6and decomposition of PVDF,and the kinetics associated was described by Avrami *** interaction of Al and F is advantageous to realize the defluoridation to some *** is expected that our investigation will provide theoretical support for the large-scale recycling of spent LIBs.

关键词： Al removal F leaching Cathode powder Heating alkali leaching Leaching kinetics