Collaborative Research: CAS: Carbene-Containing Ligands on Cu and Cu3N Nanocubes: Access to Stable and Selective Electrolysis for CO2 Reduction
合作研究:CAS:Cu 和 Cu3N 纳米立方体上的含卡宾配体:获得稳定和选择性电解以还原 CO2
基本信息
- 批准号:2102245
- 负责人:
- 金额:$ 44.25万
- 依托单位:
- 依托单位国家:美国
- 项目类别:Standard Grant
- 财政年份:2021
- 资助国家:美国
- 起止时间:2021-06-01 至 2025-05-31
- 项目状态:未结题
- 来源:
- 关键词:
项目摘要
With the support of the Chemical Catalysis program in the Division of Chemistry, Professors He and Ung at the University of Connecticut and Professor Sun at Brown University are designing new hybrid materials for selective electrochemical activation of carbon dioxide (CO2). The team will utilize synthetic polymers to coat and protect copper-based catalysts, allowing the resulting hybrid materials to be more robust and efficient for CO2 electroreduction to yield value-added hydrocarbon products. The use of renewable electricity to convert CO2 to useful chemical products is likely to be an important component of sustainability. This collaborative project will involve undergraduate, graduate, and postgraduate researchers from two universities, and will utilize each groups’ expertise in polymer, nanomaterial, organometallic, surface science, and electrochemistry. The results obtained from this project will be disseminated to science and engineering students through joint meetings, courses, undergraduate research activities, and outreach activities. The PIs are collaborating with local high schools and outreach programs in the southern New England region to attract students into studies and potential career paths in STEM (science, technology, engineering and mathematics) fields.With the support of the Chemical Catalysis program in the Division of Chemistry, Professors He and Ung at the University of Connecticut and Professor Sun at Brown University are studying new Cu-based nanocubes functionalized with synthetic polymer ligands toward stable and selective electroreduction of CO2. The central hypothesis of this proposal is twofold: i) the incorporation of Cu-based nanocubes with rationally designed synthetic polymers to prevent interparticle coalescence and surface corrosion during electroreduction, and ii) hydrophobic polymer ligands to control the microenvironment of nanocubes and improve the selectivity of nanocubes. Polymer ligands terminated with N-heterocyclic carbenes (NHCs) will be anchored on Cu, copper nitride (Cu3N) and core-shell Cu/Cu3N nanocubes through stable NHC-Cu bonds. Those nanocubes have maximum (100) surface exposure to efficiently promote C-C coupling and form C2+ hydrocarbon products. Polymer NHC ligands will balance the localized proton concentration nearby the surface of nanocubes through control over polymer chain lengths and hydrophobicity to achieve maximum catalytic proton-assisted CO2 reduction to C-C coupling products and minimize proton reduction reaction. The Cu-NHC bond stability and the structural integrity of polymer-grafted Cu and Cu3N nanocubes will be probed using in situ spectroscopies and microscopies. The polymer chain length dependent diffusion properties will be quantitatively measured and correlated to the catalytic performance of Cu and Cu3N nanocubes. The successful demonstration of the active and efficient polymer NHC-Cu nanocubes for CO2 electroreduction also allows tackling more broadly the long-term stability issues of all other cathodic nanocatalysts to improve the sustainability of electroreduction.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.
在化学系化学催化项目的支持下,康涅狄格大学的He和Ung教授以及布朗大学的Sun教授正在设计用于选择性电化学激活二氧化碳(CO2)的新型杂化材料。该团队将利用合成聚合物来覆盖和保护铜基催化剂,从而使所产生的混合材料对于二氧化碳电还原产生增值碳氢化合物产品更加坚固和高效。利用可再生电力将二氧化碳转化为有用的化学产品很可能是可持续发展的一个重要组成部分。这个合作项目将包括来自两所大学的本科生、研究生和研究生研究人员,并将利用每个小组在聚合物、纳米材料、有机金属、表面科学和电化学方面的专业知识。该项目的成果将通过联合会议、课程、本科生研究活动和外展活动向理工科学生传播。PI正在与新英格兰南部地区的当地高中和外展项目合作,以吸引学生进入STEM(科学、技术、工程和数学)领域的研究和潜在的职业道路。在化学系化学催化项目的支持下,康涅狄格大学的何教授和吴教授以及布朗大学的孙教授正在研究新的铜基纳米立方体,这些纳米立方体带有合成聚合物配体,旨在稳定和选择性地电减少二氧化碳。这一提议的中心假设有两个:i)将铜基纳米立方体与合理设计的合成聚合物结合,以防止电还原过程中的颗粒间结合和表面腐蚀;ii)疏水聚合物配体,以控制纳米立方体的微环境,提高纳米立方体的选择性。以N-杂环卡宾(NHCS)封端的聚合物配体将通过稳定的NHC-Cu键固定在铜、氮化铜(Cu3N)和核壳结构的Cu/Cu3N纳米立方体上。这些纳米立方体具有最大的(100)表面暴露,可以有效地促进C-C偶联并形成C2+烃产品。聚合物NHC配体将通过控制聚合物链长和疏水性来平衡纳米立方体表面附近的局部质子浓度,以实现最大限度地催化质子辅助二氧化碳还原为C-C偶联产物,并最大限度地减少质子还原反应。用原位光谱和显微镜研究了聚合物接枝铜和铜纳米立方体的铜-NHC键的稳定性和结构完整性。聚合物链长相关的扩散性能将被定量测量,并与铜和Cu3N纳米立方体的催化性能相关联。活性和高效的聚合物NHC-铜纳米立方体用于二氧化碳电还原的成功展示还允许更广泛地解决所有其他阴极纳米催化剂的长期稳定性问题,以提高电还原的可持续性。该奖项反映了NSF的法定使命,并通过使用基金会的智力优势和更广泛的影响审查标准进行评估,被认为值得支持。
项目成果
期刊论文数量(4)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Patchy metal nanoparticles with polymers: controllable growth and two-way self-assembly
具有聚合物的片状金属纳米颗粒:可控生长和双向自组装
- DOI:10.1039/d2nr01221a
- 发表时间:2022
- 期刊:
- 影响因子:6.7
- 作者:Duan, Hanyi;Malesky, Tessa;Wang, Janet;Liu, Chung-Hao;Tan, Haiyan;Nieh, Mu-Ping;Lin, Yao;He, Jie
- 通讯作者:He, Jie
Recent advances in CO 2 capture and reduction
CO 2 捕获和还原的最新进展
- DOI:10.1039/d2nr02894h
- 发表时间:2022
- 期刊:
- 影响因子:6.7
- 作者:Wei, Kecheng;Guan, Huanqin;Luo, Qiang;He, Jie;Sun, Shouheng
- 通讯作者:Sun, Shouheng
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Jie He其他文献
Cu2O/BiVO4 heterostructures: synthesis and application in simultaneous photocatalytic oxidation of organic dyes and reduction of Cr(VI) under visible light
Cu2O/BiVO4异质结构:可见光下同步光催化氧化有机染料和还原Cr(VI)的合成及其应用
- DOI:
10.1016/j.cej.2014.06.031 - 发表时间:
2014-11 - 期刊:
- 影响因子:15.1
- 作者:
Qing Yuan;Lang Chen;Miao Xiong;Jie He;Sheng-Lian Luo;Chak-Tong Au;Shuang-Feng Yin - 通讯作者:
Shuang-Feng Yin
The screening value of mammography for breast cancer : an overview of 22 systematic reviews with evidence mapping (Preprint)
乳房 X 光检查对乳腺癌的筛查价值:22 项系统评价与证据图谱概述(预印本)
- DOI:
- 发表时间:
2020 - 期刊:
- 影响因子:0
- 作者:
Jiyuan Shi;Jiang Li;Lili Zhang;Ya Gao;Yamin Chen;Liang Zhao;Yi;Wanqing Chen;Jinhui Tian;Ni Li;Jie He - 通讯作者:
Jie He
Shape-based reconstruction for transrectal diffuse optical tomography monitoring of photothermal focal therapy of prostate cancer: simulation studies
基于形状的重建用于前列腺癌光热局部治疗的经直肠扩散光学断层扫描监测:模拟研究
- DOI:
- 发表时间:
2017 - 期刊:
- 影响因子:3.5
- 作者:
R. Weersink;Sahil Chaudhary;Kenwrick Mayo;Jie He;B. Wilson - 通讯作者:
B. Wilson
Synthesis and photoluminescence properties of Y1-x(P0.6V0.4)O4:xEu3+ red-emitting phosphors
Y1-x(P0.6V0.4)O4:xEu3红光荧光粉的合成及光致发光性能
- DOI:
10.1007/s10854-017-7964-5 - 发表时间:
2018 - 期刊:
- 影响因子:0
- 作者:
Yalin Xu;Bing Teng;Degao Zhong;Liang Yang;Jie He;Yao Meng;Min Zhu;Jie Tang - 通讯作者:
Jie Tang
Base Metal-Controlled Chemodivergent Cyclization of Propargylamines for the Atom-Economic Synthesis of Nitrogen Heterocycles.
贱金属控制的炔丙胺化学发散环化用于氮杂环的原子经济合成。
- DOI:
- 发表时间:
2023 - 期刊:
- 影响因子:5.2
- 作者:
Hui Zhang;You Zi;Chenhui Cao;Weichun Huang;Aiwei Jiang;Chaowu Lu;Jie He;Yanfeng Tang;Zheng - 通讯作者:
Zheng
Jie He的其他文献
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{{ truncateString('Jie He', 18)}}的其他基金
Collaborative Research: SUSCHEM: Engineering Polymer-Nanocatalyst Membranes for Direct Capture of CO2 and Electrochemical Conversion to C2+ Liquid Fuel
合作研究:SUSCHEM:用于直接捕获 CO2 和电化学转化为 C2 液体燃料的工程聚合物纳米催化剂膜
- 批准号:
2324346 - 财政年份:2023
- 资助金额:
$ 44.25万 - 项目类别:
Standard Grant
CAREER: Hydrological Sensitivity Across Timescales
职业:不同时间尺度的水文敏感性
- 批准号:
2047270 - 财政年份:2021
- 资助金额:
$ 44.25万 - 项目类别:
Standard Grant
SusChEM: C-H Bond Electroactivation of Nonpolar Organic Substrates in Water: Enzyme-Mediated Reaction Pathways in Microemulsions
SusChEM:水中非极性有机底物的 C-H 键电活化:微乳液中酶介导的反应途径
- 批准号:
2035669 - 财政年份:2021
- 资助金额:
$ 44.25万 - 项目类别:
Standard Grant
EAGER: Collaborative Research: Hybrid Quantum Dot-Metal Nanocrystals for Photoreduction of CO2: Synthesis, Spectroscopy and Catalysis
EAGER:合作研究:用于二氧化碳光还原的混合量子点金属纳米晶体:合成、光谱学和催化
- 批准号:
1936228 - 财政年份:2019
- 资助金额:
$ 44.25万 - 项目类别:
Standard Grant
Collaborative Research: Solar-Driven Hydrogenation of CO2 using Hierarchically Porous TiO2 with Spatially Isolated Au and Pt Nanoparticles
合作研究:利用分级多孔 TiO2 与空间隔离的 Au 和 Pt 纳米粒子进行太阳能驱动的 CO2 氢化
- 批准号:
1705566 - 财政年份:2017
- 资助金额:
$ 44.25万 - 项目类别:
Standard Grant
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