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学者姓名：刘哲源
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Abstract ：
Doping is a recognized method for enhancing catalytic performance. The introduction of strains is a common consequence of doping, although it is often overlooked. Differentiating the impact of doping and strain on catalytic performance poses a significant challenge. In this study, Cu-doped Bi catalysts with substantial tensile strain are synthesized. The synergistic effects of doping and strain in bismuth result in a remarkable CO2RR performance. Under optimized conditions, Cu-1/6-Bi demonstrates exceptional formate Faradaic efficiency (>95%) and maintains over 90% across a wide potential window of 900 mV. Furthermore, it delivers an industrial-relevant partial current density of -317 mA cm(-2) at -1.2 V-RHE in a flow cell, while maintaining its selectivity. Additionally, it exhibits exceptional long-term stability, surpassing 120 h at -200 mA cm(-2). Through experimental and theoretical mechanistic investigations, it has been determined that the introduction of tensile strain facilitates the adsorption of *CO2, thereby enhancing the reaction kinetics. Moreover, the presence of Cu dopants and tensile strain further diminishes the energy barrier for the formation of *OCHO intermediate. This study not only offers valuable insights for the development of effective catalysts for CO2RR through doping, but also establishes correlations between doping, lattice strains, and catalytic properties of bismuth catalysts.
Keyword ：
bismuth bismuth CO2 reduction CO2 reduction doping doping strain strain synergistic effect synergistic effect
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| GB/T 7714 | Wei, Yang , Xu, Xin , Shi, Dehuan et al. Synergistic Effects of Doping and Strain in Bismuth Catalysts for CO2 Electroreduction [J]. | SMALL , 2024 . |
| MLA | Wei, Yang et al. "Synergistic Effects of Doping and Strain in Bismuth Catalysts for CO2 Electroreduction" . | SMALL (2024) . |
| APA | Wei, Yang , Xu, Xin , Shi, Dehuan , Jiang, Yaming , Zheng, Chaoyang , Tan, Li et al. Synergistic Effects of Doping and Strain in Bismuth Catalysts for CO2 Electroreduction . | SMALL , 2024 . |
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Organic electrode materials are promising for next-generation energy storage materials due to their environmental friendliness and sustainable renewability. However, problems such as their high solubility in electrolytes and low intrinsic conductivity have always plagued their further application. Polymerization to form conjugated organic polymers can not only inhibit the dissolution of organic electrodes in the electrolyte, but also enhance the intrinsic conductivity of organic molecules. Herein, we synthesized a new conjugated organic polymer (COPs) COP500-CuT2TP (poly [5,10,15,20-tetra(2,2 '-bithiophen-5-yl) porphyrinato] copper (II)) by electrochemical polymerization method. Due to the self-exfoliation behavior, the porphyrin cathode exhibited a reversible discharge capacity of 420 mAh g-1, and a high specific energy of 900 Wh Kg-1 with a first coulombic efficiency of 96 % at 100 mA g-1. Excellent cycling stability up to 8000 cycles without capacity loss was achieved even at a high current density of 5 A g-1. This highly conjugated structure promotes COP500-CuT2TP combined high energy density, high power density, and good cycling stability, which would open new opportunity for the designable and versatile organic electrodes for electrochemical energy storage. A new porphyrin conjugated polymer cathode, COP500-CuT2TP is achieved under electrochemical polymerization. Self-exfoliation of polymer cathode promotes charge storage, leading to a specific capacity of 420 mAh g-1 and 900 Wh Kg-1. Excellent cycling stability up to 8000 cycles at 5 A g-1 is achieved. Mechanistic insights by combining experimental and computational investigations supports the charge storage performance. image
Keyword ：
conjugated organic polymers conjugated organic polymers lithium-ion batteries lithium-ion batteries porphyrin porphyrin thiophene thiophene
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| GB/T 7714 | Wu, Xing , Zhou, Wang , Ye, Chao et al. Porphyrin-Thiophene Based Conjugated Polymer Cathode with High Capacity for Lithium-Organic Batteries [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (14) . |
| MLA | Wu, Xing et al. "Porphyrin-Thiophene Based Conjugated Polymer Cathode with High Capacity for Lithium-Organic Batteries" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 14 (2024) . |
| APA | Wu, Xing , Zhou, Wang , Ye, Chao , Zhang, Jiahao , Liu, Zheyuan , Yang, Chengkai et al. Porphyrin-Thiophene Based Conjugated Polymer Cathode with High Capacity for Lithium-Organic Batteries . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (14) . |
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As an important interaction among organic cations containing aromatic rings, the pi-pi stacking interaction is a crucial factor determining the crystal structure of organic-inorganic hybrid metal halides (OIMHs). However, the relationship between pi-pi interaction and optical properties of luminescent OIMHs is yet to be studied. (C10H10N2)Cd1-xZnxCl4 (23-Cd1-xZnxCl4) crystals with 0D structures are synthesized by using optically active 2,3 '-bipyridine as the organic ligand. When x <= 0.2, there is no pi-pi interaction among 2,3 '-bipyridinium cations in 23-Cd1-xZnxCl4 crystals. When x > 0.2, pi-pi interaction among organic cations occurs and enhances as the Zn2+ content increases. The tailoring of the pi-pi interaction endows 23-Cd1-xZnxCl4 with tunable light emitting properties, resulting in a broad band emission involving blue and orange species. The blue emission dominates when there is no pi-pi interaction, while the orange emission enhances and finally becomes dominant as the strength of pi-pi interaction increases. The pi-pi interaction promotes the energy transfer from the higher energy valley to the lower one of the S-1 state of the organic cation, resulting in the enhancement of orange emission. Notably, the 23-ZnCl crystal exhibits a photo-luminescence quantum yield (PLQY) of 32%. This is the highest reported value to date among the Zn-based OIMHs, which have optical emission originating from the organic component. The mechanism of pi-pi stacking induced tunable light emission revealed in our work provides new guidance for the design of luminescent OIMHs.
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| GB/T 7714 | Zhang, Qi , Lin, Xinyi , Guo, Shanji et al. Tailoring the π-π stacking interaction among organic cations in hybrid metal halide crystals towards tunable light emission [J]. | JOURNAL OF MATERIALS CHEMISTRY C , 2024 , 12 (19) : 7053-7061 . |
| MLA | Zhang, Qi et al. "Tailoring the π-π stacking interaction among organic cations in hybrid metal halide crystals towards tunable light emission" . | JOURNAL OF MATERIALS CHEMISTRY C 12 . 19 (2024) : 7053-7061 . |
| APA | Zhang, Qi , Lin, Xinyi , Guo, Shanji , Zhang, Yaqing , Jiang, Yan , Zhang, Wei et al. Tailoring the π-π stacking interaction among organic cations in hybrid metal halide crystals towards tunable light emission . | JOURNAL OF MATERIALS CHEMISTRY C , 2024 , 12 (19) , 7053-7061 . |
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The serious dendrite formation and safety hazards associated with side reactions hinder the practical application of lithium metal batteries. A molecular customization strategy based on both physical and chemical properties is reported. A copolymer of acrylamide and hexafluorobutyl acrylate molecules is used as an artificial solid electrolyte interface(ASEI) for lithium metal to achieve dynamic interface protection during cycling. The amide group serves as the rigid unit, while the hexafluorobutyl group serves as the flexible unit, and imparts excellent mechanical properties to the copolymer. Synergistically abundant CF bonds exhibit excellent water and oxygen resistance and have good electrolyte affinity. The ester and amide groups serve as amphiphilic sites for Li+ and PF6-, regulating the ion flux at the interface and achieving dendrite-free lithium deposition. During cycling, the organic-inorganic composite SEI dynamically evolves to safeguard the lithium metal, preventing undue electrolyte consumption. The copolymer achieves stable cycling for 1500 and 950 h at 1 and 2 mA cm-2, respectively. It demonstrates excellent performance with LiNi0.8Co0.1Mn0.1O2 and LiFePO4 cathodes. This study introduces a new approach to designing polymers at the molecular level to optimize the physical properties/chemical activity of lithium metal interfaces. The serious dendrite formation and safety hazards associated with side reactions hinder the practical application of lithium metal batteries. A molecular customization polymer based on physicochemical properties as ASEI is reported. The copolymer has excellent mechanical properties and water and oxygen resistance. The ester and amide groups serve as amphiphilic sites, regulating the ion flux and achieving dendrite-free lithium deposition. image
Keyword ：
binary copolymer binary copolymer dendrite suppression dendrite suppression interface engineering interface engineering lithium metal anode lithium metal anode
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| GB/T 7714 | Luo, Jing , Huang, Qinzhui , Shi, Dehuan et al. Dynamic Interfacial Protection via Molecularly Tailored Copolymer for Durable Artificial Solid Electrolyte Interphase in Lithium Metal Batteries [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 . |
| MLA | Luo, Jing et al. "Dynamic Interfacial Protection via Molecularly Tailored Copolymer for Durable Artificial Solid Electrolyte Interphase in Lithium Metal Batteries" . | ADVANCED FUNCTIONAL MATERIALS (2024) . |
| APA | Luo, Jing , Huang, Qinzhui , Shi, Dehuan , Qiu, Yanbin , Zheng, Xinyu , Yang, Sisheng et al. Dynamic Interfacial Protection via Molecularly Tailored Copolymer for Durable Artificial Solid Electrolyte Interphase in Lithium Metal Batteries . | ADVANCED FUNCTIONAL MATERIALS , 2024 . |
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The practical application of Zn-ion batteries (ZIBs) faces several challenges, particularly regarding poor reversibility and the reactivity of water in the electrolytes across a wide temperature range. Herein, this study presents the design of a ternary electrolyte with significant intermolecular interactions based on tetrahydrofurfuryl alcohol (THFA), H2O, and Zn(OTf)(2) to address these challenges from -40 to 60 C-degrees. The ether alcohol compound THFA effectively mitigates the side reactions about water, by disrupting and suppressing the reactivity of the dominant water-based clusters. Through experimental and theoretical investigations, the structural and mechanistic insights of ternary solvation clusters are uncovered. The hydrogen-bond-induced interactions of THFA facilitate the participation of OTf- in solvation clusters and bidentate chelation coordination with Zn2+ ensures the formation of lean-water solvation clusters. Furthermore, the interfacial electrochemistry on the Zn surface is also regulated to exhibit a preferential layer-by-layer (0 0 2) oriented deposition with a stable solid electrolyte interface (SEI). As a result, The Zn||VO2 battery using ternary electrolyte maintains a capacity of 237.5 mAh g(-1) with an 86.71% retention after 500 cycles at 60 C-degrees and 3 A g(-1), while it exhibits stable cycle even at -40 C-degrees over 200 cycles with almost no capacity decrease.
Keyword ：
bidentate ligands bidentate ligands dual hydrogen bonds dual hydrogen bonds solid electrolyte interface solid electrolyte interface ternary electrolytes ternary electrolytes wide-temperature wide-temperature Zn (002) oriented deposition Zn (002) oriented deposition
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| GB/T 7714 | Qiu, Yanbin , Zheng, Xinyu , Zhang, Ran et al. Boosting Zinc-Ion Batteries with Innovative Ternary Electrolyte for Enhanced Interfacial Electrochemistry and Temperature-Resilient Performance [J]. | ADVANCED FUNCTIONAL MATERIALS , 2023 , 34 (4) . |
| MLA | Qiu, Yanbin et al. "Boosting Zinc-Ion Batteries with Innovative Ternary Electrolyte for Enhanced Interfacial Electrochemistry and Temperature-Resilient Performance" . | ADVANCED FUNCTIONAL MATERIALS 34 . 4 (2023) . |
| APA | Qiu, Yanbin , Zheng, Xinyu , Zhang, Ran , Lin, Qingqing , Li, Mengchao , Luo, Jing et al. Boosting Zinc-Ion Batteries with Innovative Ternary Electrolyte for Enhanced Interfacial Electrochemistry and Temperature-Resilient Performance . | ADVANCED FUNCTIONAL MATERIALS , 2023 , 34 (4) . |
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Extensive fast-neutron-based applications and radiation monitoring are inseparable from fast-neutron detection, but the interference of accompanying y rays requires fast-neutron/y discrimination (FNGD). Organic single-crystal scintillators (OSCSs) generate fast-neutron -induced delayed fluorescence and y-induced prompt fluorescence (PF), which can be discriminated by one-step pulse-shape discrimination (PSD). However, PSD cannot identify neutron-induced PF, introducing errors in neutron counting. Here, we report a dual-discrimination approach for accurate fast-neutron detection using y-ray-insensitive tetraphenylethylene (TPE). In contrast to previous OSCSs, TPE realizes FNGD by PSD and pulse-height discrimination (PHD), since it simultaneously exhibits disparities in shape and pulse height under neutron and y irradiation. PHD enables secondary FNGD from PF, significantly increasing neutron counts. The improved FNGD method based on TPE reveals a high figure of merit (FoM = 2.4) and count rate of neutrons (35.5%). Our research provides new ideas and avail-able materials for high-efficiency FNGD, promoting the applications of fast neutrons.
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| GB/T 7714 | Sun, Qisheng , Hao, Zirui , Li, Jing et al. Dual discrimination of fast neutrons from strong y noise using organic single-crystal scintillator [J]. | MATTER , 2023 , 6 (1) : 274-284 . |
| MLA | Sun, Qisheng et al. "Dual discrimination of fast neutrons from strong y noise using organic single-crystal scintillator" . | MATTER 6 . 1 (2023) : 274-284 . |
| APA | Sun, Qisheng , Hao, Zirui , Li, Jing , Liu, Zheyuan , Wang, Hongwei , Zhang, Xiaotao et al. Dual discrimination of fast neutrons from strong y noise using organic single-crystal scintillator . | MATTER , 2023 , 6 (1) , 274-284 . |
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利用太阳能和半导体催化材料将CO_2还原为具有高附加值的含碳化学品为解决能源危机等问题提供了一个有前景的解决方案.目前半导体光催化CO_2还原的效率仍然很低,这主要是光激发的载流子复合严重等问题导致的.探索有效策略来增强半导体光催化材料光生电荷分离和传输性能被认为是提高CO_2还原效率的关键之一.设计制备具有定向电荷传输性能的光催化材料将有助于抑制光生电荷复合,从而实现高效光催化性能.线型共轭有机聚合物具有直链状结构、明晰和多样的元素组成、良好的水热稳定性等优点在光催化领域受到持续的关注和研究.本文通过均苯四甲酸二酐和二胺单体的缩合反应制备了三例晶态线型共轭聚酰亚胺材料用于光催化CO_2还原.利用粉末X射线衍射、傅里叶红外光谱、扫描电子显微镜、透射电子显微镜、紫外可见吸收光谱和气体吸附测试等对合成的聚酰亚胺的晶态结构、光吸收性质、形貌结构和孔结构等进行了表征.利用光电化学、电子顺磁共振波普分析、电位分析和密度泛函理论计算等研究了构筑单元的电子推拉效应对聚合物电荷分离及催化性能的影响.结果表明,三种结晶型聚酰亚胺均对CO_2具有良好的吸附能力且满足光催化CO_2还原电势的能带结构要求.光生载流子的复合程度随着重复结构单元偶极距的增强而降低,其中基于苯并噻吩砜的晶态线型聚酰亚胺(CLP-CS)具有最优的载流子分离能力.在光催化CO_2还原反应中, CLP-CS表现出高达1700μmol h~(-1) gcat~(-1)的CO析出效率和90%的选择性.CLP-CS在高低温和紫外灯照射等极端条件下,仍保持良好的结构稳定性和催化活性.实验发现,聚合物的CO_2还原活性与重复结构单元的偶极距及方向密切有关.局部结构的不对称性,扩大了分子偶极,增强了材料的内建电场驱动力.此外,长程有序的线型结构为光生电荷传输提供了快速迁移通道,促进了载流子迁移.综上,本文报道了基于晶态线型聚合物的光催化体系,为实现光生电荷定向传输和开发高效光催化材料提供了途径.
Keyword ：
二氧化碳还原 二氧化碳还原 光催化 光催化 电子定向转移 电子定向转移 结晶聚合物 结晶聚合物 聚酰亚胺 聚酰亚胺
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| GB/T 7714 | 李慧珍 , 陈艳蕾 , 牛青 et al. 具有定向电荷传递能力的晶态线型聚酰亚胺材料驱动光催化CO_2还原（英文） [J]. | Chinese Journal of Catalysis , 2023 , 49 (06) : 152-159 . |
| MLA | 李慧珍 et al. "具有定向电荷传递能力的晶态线型聚酰亚胺材料驱动光催化CO_2还原（英文）" . | Chinese Journal of Catalysis 49 . 06 (2023) : 152-159 . |
| APA | 李慧珍 , 陈艳蕾 , 牛青 , 王小凤 , 刘哲源 , 毕进红 et al. 具有定向电荷传递能力的晶态线型聚酰亚胺材料驱动光催化CO_2还原（英文） . | Chinese Journal of Catalysis , 2023 , 49 (06) , 152-159 . |
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Abstract ：
利用太阳能和半导体催化材料将CO2还原为具有高附加值的含碳化学品为解决能源危机等问题提供了一个有前景的解决方案.目前半导体光催化CO2还原的效率仍然很低,这主要是光激发的载流子复合严重等问题导致的.探索有效策略来增强半导体光催化材料光生电荷分离和传输性能被认为是提高CO2还原效率的关键之一.设计制备具有定向电荷传输性能的光催化材料将有助于抑制光生电荷复合,从而实现高效光催化性能.线型共轭有机聚合物具有直链状结构、明晰和多样的元素组成、良好的水热稳定性等优点在光催化领域受到持续的关注和研究.本文通过均苯四甲酸二酐和二胺单体的缩合反应制备了三例晶态线型共轭聚酰亚胺材料用于光催化CO2还原.利用粉末X射线衍射、傅里叶红外光谱、扫描电子显微镜、透射电子显微镜、紫外可见吸收光谱和气体吸附测试等对合成的聚酰亚胺的晶态结构、光吸收性质、形貌结构和孔结构等进行了表征.利用光电化学、电子顺磁共振波普分析、电位分析和密度泛函理论计算等研究了构筑单元的电子推拉效应对聚合物电荷分离及催化性能的影响.结果表明,三种结晶型聚酰亚胺均对CO2具有良好的吸附能力且满足光催化CO2还原电势的能带结构要求.光生载流子的复合程度随着重复结构单元偶极距的增强而降低,其中基于苯并噻吩砜的晶态线型聚酰亚胺(CLP-CS)具有最优的载流子分离能力.在光催化CO2还原反应中,CLP-CS表现出高达1700 μmolh-1gcat-1的CO析出效率和90％的选择性.CLP-CS在高低温和紫外灯照射等极端条件下,仍保持良好的结构稳定性和催化活性.实验发现,聚合物的CO2还原活性与重复结构单元的偶极距及方向密切有关.局部结构的不对称性,扩大了分子偶极,增强了材料的内建电场驱动力.此外,长程有序的线型结构为光生电荷传输提供了快速迁移通道,促进了载流子迁移.综上,本文报道了基于晶态线型聚合物的光催化体系,为实现光生电荷定向传输和开发高效光催化材料提供了途径.
Keyword ：
二氧化碳还原 二氧化碳还原 光催化 光催化 电子定向转移 电子定向转移 结晶聚合物 结晶聚合物 聚酰亚胺 聚酰亚胺
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| GB/T 7714 | 李慧珍 , 陈艳蕾 , 牛青 et al. 具有定向电荷传递能力的晶态线型聚酰亚胺材料驱动光催化CO2还原 [J]. | 催化学报 , 2023 , 49 (6) : 152-159 . |
| MLA | 李慧珍 et al. "具有定向电荷传递能力的晶态线型聚酰亚胺材料驱动光催化CO2还原" . | 催化学报 49 . 6 (2023) : 152-159 . |
| APA | 李慧珍 , 陈艳蕾 , 牛青 , 王小凤 , 刘哲源 , 毕进红 et al. 具有定向电荷传递能力的晶态线型聚酰亚胺材料驱动光催化CO2还原 . | 催化学报 , 2023 , 49 (6) , 152-159 . |
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The achievement of artificial photosynthesis relies on successful water oxidation and a detailed mechanistic understanding. Here, we demonstrate a photoinduced hydration pathway for O2 evolution from water oxidation over an iminelinked covalent organic framework (COF) comprising electron rich benzotrithiophene and electron-deficient benzothiadiazole units with atomically chelated Co sites. The experimental and theoretical results suggest that the water oxidation starts with the photoinduced hydration of imine groups. The subsequent oxidative deprotonation and intramolecular hydroxyl attack lead to O-O bond formation. The hydration path significantly averages the energy barriers of water oxidation, thus promoting O2 evolution. Inspired by this fact, we fabricate a COF-based heterostructure, which realizes overall water splitting with H2 and O2 evolution rates of 450 and 212 mu mol center dot g-1 h-1, respectively.
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| GB/T 7714 | He, Yajun , Liu, Guoyu , Liu, Zheyuan et al. Photoinduced Hydration Boosts O2 Evolution on Co-Chelating Covalent Organic Framework [J]. | ACS ENERGY LETTERS , 2023 : 1857-1863 . |
| MLA | He, Yajun et al. "Photoinduced Hydration Boosts O2 Evolution on Co-Chelating Covalent Organic Framework" . | ACS ENERGY LETTERS (2023) : 1857-1863 . |
| APA | He, Yajun , Liu, Guoyu , Liu, Zheyuan , Bi, Jinhong , Yu, Yan , Li, Liuyi . Photoinduced Hydration Boosts O2 Evolution on Co-Chelating Covalent Organic Framework . | ACS ENERGY LETTERS , 2023 , 1857-1863 . |
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High performance lithium metal anode is of great importance to achieve batteries with high energy density. Due to the intrinsic high reactivity of Li metal anode and the insufficient understanding of lithium redox at the Li/ electrolyte interface, the fast and dendrite-free Li metal deposition still remains a grand challenge. In this work, we accelerate Li+/Li redox through the regulation of the electric double layer (EDL), in which 2-Mercaptopyri-dine (2-MP), a conjugated weak-base molecule with stable electrochemical properties, can be specifically adsorbed on Li metal surface and promote charge transfer. It fundamentally avoided the formation of Li metal dendrites and enabled fast Li plating/stripping process, leading to uniform Li deposition as well as superior cycling performances of batteries. This work provides a significant contribution to the understanding of battery chemistry at the electrode/electrolyte interface.
Keyword ：
2-Mercaptopyridine 2-Mercaptopyridine Dendrite Dendrite Electric double layer Electric double layer Li metal anode Li metal anode Lithium metal batteries Lithium metal batteries
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| GB/T 7714 | Zhou, Tianyi , Shi, Dehuan , Wang, Qian et al. Accelerating Li plus /Li redox through the regulation of the electric double layer for efficient lithium metal anodes [J]. | CHEMICAL ENGINEERING JOURNAL , 2023 , 468 . |
| MLA | Zhou, Tianyi et al. "Accelerating Li plus /Li redox through the regulation of the electric double layer for efficient lithium metal anodes" . | CHEMICAL ENGINEERING JOURNAL 468 (2023) . |
| APA | Zhou, Tianyi , Shi, Dehuan , Wang, Qian , Yang, Chengkai , Wang, Xiaolong , Wu, Kai et al. Accelerating Li plus /Li redox through the regulation of the electric double layer for efficient lithium metal anodes . | CHEMICAL ENGINEERING JOURNAL , 2023 , 468 . |
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