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Carbon-Dot-Enhanced Electrocatalytic Hydrogen Evolution

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Accounts of Materials Research 2022年第3期3卷 319-330页

作者： Han Wu Siyu Lu Bai Yang Green Catalysis Center and College of Chemistry Zhengzhou UniversityZhengzhou 450001P.R.China State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012P.R.China

CONSPECTUS:Hydrogen evolution by the electrolysis of water is an important energy conversion process,especially for some intermittent energy systems.However,its practical applicability is limited by its low energy-conversion efficiency and the need for expensive electrocatalysts.In response,carbon-based nanocomposites have gained substantial interest as promising alternatives to the currently used precious metal catalysts.Among them,carbon dots(CDs)have exhibited many outstanding features,including flexible composition,high conductivity,good dispersion,and strong metal coordination.The past decade has seen remarkable advances in CD-based electrocatalysts for hydrogen evolution,where CDs and their derived hybrids have shown impressive performance and indispensable prospects for future hydrogen utilization.However,the widespread use of CD-based electrocatalysts still requires the development of high-quality CDs and advanced synthesis strategies.New assessment techniques are also required to elucidate the unique functions of CDs in composition regulation,structure fabrication,surface modification,and host−guest interactions in electrocatalysts and ultimately to establish the relationships among structure,composition,and activity.

关键词： gained catalytic Hydrogen

Progress on the mechanisms of Ru-based electrocatalysts for the oxygen evolution reaction in acidic media

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Journal of Energy Chemistry 2023年第10期85卷 220-238,I0008页

作者： Yuanyuan Shi Han Wu Jiangwei Chang Zhiyong Tang Siyu Lu Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001HenanChina CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China

Water electrolysis using proton-exchange membranes is one of the most promising technologies for carbon-neutral and sustainable energy production.Generally,the overall efficiency of water splitting is limited by the oxygen evolution reaction(OER).Nevertheless,a trade-off between activity and stability exists for most electrocatalytic materials in strong acids and oxidizing media,and the development of efficient and stable catalytic materials has been an important focus of research.In this view,gaining in-depth insights into the OER system,particularly the interactions between reaction intermediates and active sites,is significantly important.To this end,this review introduces the fundamentals of the OER over Ru-based materials,including the conventional adsorbate evolution mechanism,lattice oxygen oxidation mechanism,and oxide path mechanism.Moreover,the up-to-date progress of representative modifications for improving OER performance is further discussed with reference to specific mechanisms,such as tuning of geometric,electronic structures,incorporation of proton acceptors,and optimization of metal-oxygen covalency.Finally,some valuable insights into the challenges and opportunities for OER electrocatalysts are provided with the aim to promote the development of next-generation catalysts with high activity and excellent stability.

关键词： Oxygen evolution reaction Ru-based electrocatalysts Acidic solutions Mechanism Proton-exchange membranes

Electrocatalytic water splitting:Mechanism and electrocatalyst design

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Nano Research 2023年第7期16卷 9142-9157页

作者： Han Wu Qiaoxian Huang Yuanyuan Shi Jiangwei Chang Siyu Lu Green Catalysis Center College of ChemistryZhengzhou UniversityZhengzhou 450001China

Hydrogen energy,a new type of clean and efficient energy,has assumed precedence in decarbonizing and building a sustainable carbon-neutral economy.Recently,hydrogen production from water splitting has seen considerable advancements owing to its advantages such as zero carbon emissions,safety,and high product purity.To overcome the large energy barrier and high cost of water splitting,numerous efficient electrocatalysts have been designed and reported.However,various difficulties in promoting the industrialization of electrocatalytic water splitting remain.Further,as high-performance electrocatalysts that satisfy industrial requirements are urgently needed,a better understanding of water-splitting systems is required.In this paper,the latest progress in water electrolysis is reviewed,and experimental evidence from in situ/operando spectroscopic surveys and computational analyses is summarized to present a mechanistic understanding of hydrogen and oxygen evolution reactions.Furthermore,some promising strategies,including alloying,morphological engineering,interface construction,defect engineering,and strain engineering for designing and synthesizing electrocatalysts are highlighted.We believe that this review will provide a knowledge-guided design in fundamental science and further inspire technical engineering developments for constructing efficient electrocatalysts for water splitting.

关键词： water splitting mechanism operando spectroscopy design strategy

Light Inducing the Geometric Conversion of NiO_(6) to Trigger a Faster Oxygen Evolution Reaction Pathway:The Coupled Oxygen Evolution Mechanism

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Energy & Environmental Materials 2023年第2期6卷 408-410页

作者： Hao Wang Siyu Lu Green Catalysis Center College of ChemistryZhengzhou UniversityZhengzhou 450001China

Developing highly active and robust oxygen evolution reaction(OER)electrocatalysts is still a critical challenge for water electrolyzers and metal-air batteries.Realizing the dynamic evolution of the intermediate and charge transfer during OER and developing a clear OER mechanism is crucial to design high-performance OER catalysts.Recently in Nature,Xue and colleagues revealed a new OER mechanism,coupled oxygen evolution mechanism(COM),which involves a switchable metal and oxygen redox under light irradiation in nickel oxyhydroxide-based materials.This newly developed mechanism requires a reversible geometric conversion between octahedron(NiO_(6))and square planar(NiO_(4))to achieve electronic states with both“metal redox”and“oxygen redox”during OER.The asymmetric structure endows NR-NiOOH with a nonoverlapping region between the dz^(2) orbitals and a_(1g)^(*)bands,which facilitate the geometric conversion and enact the COM pathway.As a result,NR-NiOOH exhibited better OER activity and stability than the traditional NiOOH.

关键词： coupled oxygen evolution mechanism geometric conversion light-induced oxygen evolution reaction

Near-infrared emissive carbon dots with 33.96% emission in aqueous solution for cellular sensing and light-emitting diodes

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Science Bulletin 2019年第17期64卷 1285-1292页

作者： Boyang Wang Jian Li Zhiyong Tang Bai Yang Siyu Lu College of Chemistry Zhengzhou University Zhengzhou 450001 China Henan Institute of Advanced Technology Zhengzhou University Zhengzhou 450001 China CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in Nanoscience National Center for Nanoscience and Technology Beijing 100190 China State Key Laboratory of Supramolecular Structure and Materials College of Chemistry Jilin University Changchun 130012 China

Near-infrared emissive carbon dots(CDs) were synthesized by hydrothermal method. The as-prepared CDs exhibited a relatively high quantum yield(QY) of 33.96% in an aqueous solution, and the peak toward the near-infrared fluorescence reached 685 nm. The CDs exhibited pH-sensitive characteristics under strong acidic conditions. Even at pH = 0, the as-prepared CDs retained a high fluorescence intensity,which proved that they possessed good acid resistance. More importantly, the CDs were sensitive to the Fe3+changes in living cells. In addition, they could also be used for white and red emissive LEDs.This discovery will expand the use of aqueous-phase high QY CDs in the field of living cell sensing and imaging.

关键词： Carbon dots Fluorescence Red emission Aqueous Cellular sensing

High production-yield solid-state carbon dots with tunable photoluminescence for white/multi-color light-emitting diodes

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Science Bulletin 2019年第23期64卷 1788-1794页

作者： Haoqiang Song Xuejian Liu Boyang Wang Zhiyong Tang Siyu Lu College of Chemistry Zhengzhou UniversityZhengzhou 450001China Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou 450001China CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China

Plastic waste is generally resistant to natural degradation and has become a major environmental pollution problem globally. The pollution of ecosystems seriously affects the health and survival of organisms,including humans. Much attention has been paid to finding suitable ways to convert plastic waste into high-value-added carbon materials. To this end, we report the high production yield(60%–85%) of carbon dots(CDs) for solid-state fluorescence(SSF) obtained by a one-step solvothermal method using waste expanded polystyrene as the precursor. The SSF mechanism of the CDs was also explored. Their emission wavelength, with a large full width at half maximum of 150–200 nm, exhibited tunable photoluminescence from white to yellow and orange. CDs powder was used to fabricate single-component white and multi-colour light-emitting diodes on UV chips. Overall, plastic waste was converted into tunable solid-state fluorescent CDs powder, which has promising applications in carbon-based lighting, by a simple solvothermal method that provides a viable method for recycling plastic waste.

关键词： Carbon dots High production yield Solid-state fluorescence Light-emitting dots

Video-based body geometric aware network for 3D human pose estimation

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Optoelectronics Letters 2022年第5期18卷 313-320页

作者： LI Chaonan LIU Sheng YAo lu ZOU siyu College of Computer Science and Technology Zhejiang University of TechnologyHangzhou 310023Chiana

Three-dimensional human pose estimation(3 D HPE) has broad application prospects in the fields of trajectory prediction, posture tracking and action analysis. However, the frequent self-occlusions and the substantial depth ambiguity in two-dimensional(2 D) representations hinder the further improvement of accuracy. In this paper, we propose a novel video-based human body geometric aware network to mitigate the above problems. Our network can implicitly be aware of the geometric constraints of the human body by capturing spatial and temporal context information from 2 D skeleton data. Specifically, a novel skeleton attention(SA) mechanism is proposed to model geometric context dependencies among different body joints, thereby improving the spatial feature representation ability of the network. To enhance the temporal consistency, a novel multilayer perceptron(MLP)-Mixer based structure is exploited to comprehensively learn temporal context information from input sequences. We conduct experiments on publicly available challenging datasets to evaluate the proposed approach. The results outperform the previous best approach by 0.5 mm in the Human3.6 m dataset. It also demonstrates significant improvements in Human Eva-I dataset.

关键词： network geometric estimation

Advances, opportunities, and challenge for full-color emissive carbon dots

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Chinese Chemical Letters 2022年第2期33卷 613-625页

作者： Xin Yang Xue Li Boyang Wang Lin Ai Guoping Li Bai Yang Siyu Lu Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001China State Key Laboratory of Bio-Fibers and Eco-Textiles Qingdao UniversityQingdao 132101China State Key Laboratory of Superhard Materials College of PhysicsJilin UniversityChangchun 130012China State Key Lab of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China

Carbon dots(CDs), novel luminescent zero-dimensional carbon nanomaterials, have been widely applied due to their low toxicity, optimal optical properties, and easy modification. However, the current controllable equipment and mechanism explanation of CDs are relatively vague and require urgent resolution.Full-color emission CDs, an essential CDs category, have attracted people’s attention given their light and color-tunable properties. In addition to a wider range of biological and optoelectronic device applications, full-color emission CDs have similar structures and significantly affected the fluorescence mechanism of CDs. At present, few studies have reported on the summary research of CDs emitted by its full color, which greatly limits the development of CDs mechanisms and applications. As such, the present review detailed the full-color CDs development status, to which a suitable method for preparing full-color CDs was presented and the existing fluorescence emission mechanism of full-color CDs was summarized.Herein, we comprehensively introduced full-color CDs applications in biology and optoelectronics. Finally,we made an outlook on the development and potential applications of full-color CDs. The present review aims to contribute novel insights and methods for understanding full-color CDs.

关键词： Carbon dots Full-color emission Preparation Fluorescence mechanism Application

偶极-偶极相互作用诱导量子点自组装的高效发光二极管

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科学通报 2024年第11期69卷 1387-1389页

作者：卢思宇郑州大学化学学院郑州450001

量子点发光二极管(quantum dot light-emitting diodes,QD-LED)具有色域覆盖范围广、溶液加工成本低以及低电压下亮度和效率高等突出优势,是下一代显示技术的有力竞争者[1~3].外量子效率(external quantum efficiency,EQE)是QDLED走向... 详细信息

量子点发光二极管(quantum dot light-emitting diodes,QD-LED)具有色域覆盖范围广、溶液加工成本低以及低电压下亮度和效率高等突出优势,是下一代显示技术的有力竞争者[1~3].外量子效率(external quantum efficiency,EQE)是QDLED走向应用至关重要的性能指标,其中,内量子效率与外耦合效率共同决定了外量子效率.

关键词：外量子效率量子点发光二极管内量子效率耦合效率溶液加工