Spectroscopy-led Development of Organic Photocatalysts for Sustainable Energy Production

光谱主导的有机光催化剂开发用于可持续能源生产

• 批准号: RGPIN-2019-05521
• 负责人: Godin, Robert
• 金额: $ 1.75万
• 依托单位: University of British Columbia
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2022
• 资助国家: 加拿大
• 起止时间: 2022-01-01 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=761668
• 关键词: Spectroscopy; led; Development; Organic; Photocatalysts

Renewable solar energy needs to be paired with energy storage to overcome the hourly mismatch between solar energy supply and energy demands. Inspired by the natural photosynthesis of plants, solar energy can be stored in high-density chemical bonds. Solar fuels - high energy molecules generated from sunlight - can be produced by photocatalysts that drive water splitting (to make H2) or photoreduction of CO2 (to make liquid fuels). To accelerate the transition to a low-carbon society, cost-effective photocatalysts that produce solar fuels with improved efficiencies must be developed. Carbon nitride (CNx) has emerged as a leading cost-effective photocatalyst. CNx can be synthesized by simple heat treatment of inexpensive molecules and has the requisite (photo)chemical stability. High photocatalytic efficiencies (quantum yields up to 50%) for H2 photogeneration have been demonstrated using sacrificial oxidation substrates. To close the sustainable solar fuel cycle, these substrates must be replaced with H2O, the product generated when energy is released. However, H2O oxidation is more challenging. The resulting solar-to-fuel efficiency < 1% is far from the targeted commercialization barrier of 10%. My research program will develop the structure-activity relationships needed to engineer superior photocatalysts. The advanced spectroscopic technique of transient absorption spectroscopy (TAS) will shed light on the photophysics of CNx and identify the most crippling efficiency bottlenecks. The impact of energetic, structural and spatial heterogeneities on photoefficiency is poorly understood. To gain a holistic view of the key processes that determine photoactivity, my group will investigate the charge carrier dynamics of CNx modified on three different axes: (nano)morphology, chemical nature of terminal groups, and deposited redox cocatalysts. To uncover spatial heterogeneities in CNx, I will develop microsecond - second transient absorption microscopy (TAM) to map out processes such as charge trapping, charge accumulation and interfacial charge transfer. Spectroscopy will yield crucial photophysical and structural insights needed to direct synthetic modifications of photocatalysts. The synergistic spectroscopic and synthetic approach will optimize CNx morphology and internal photophysics, required for both efficient H2 production and CO2 photoreduction. My long-term vision is to take advantage of the optimized CNx photophysics to develop solar-driven carbon capture and utilization, using CNx and light to sequester CO2 within materials with long lifespans. HQP involved in the research program will gain a unique combination of synthetic, spectroscopic, communication, and management skills that make them attractive to the growing clean technology sector. HQP will contribute to the clean energy sector and the important H2 industry that will surpass US$200 Bn by the end of 2025, developing Canada's economy and helping reach lower CO2 emissions targets.

可再生太阳能需要与能源存储配对，以克服太阳能供应和能源需求之间的小时不匹配。受植物的自然光合作用的启发，太阳能可以存储在高密度的化学键中。太阳能燃料 - 由阳光产生的高能量分子 - 可以通过驱动水分（制造H2）或二氧化碳（制造液态燃料）的光催化剂产生。为了加速向低碳社会的过渡，必须开发出具有提高效率的太阳能燃料的成本效益的光催化剂。氮化碳（CNX）已成为领先的成本效益光催化剂。 CNX可以通过简单的廉价分子热处理来合成，并具有必要的（照片）化学稳定性。使用牺牲氧化底物证明了H2光学的高光催化效率（量子产量高达50％）。为了关闭可持续的太阳能燃料周期，必须将这些基材替换为H2O，这是释放能量时产生的产品。但是，H2O氧化更具挑战性。由此产生的太阳能到燃料效率<1％远非目标商业化障碍远远10％。我的研究计划将开发设计高级光催化剂所需的结构活性关系。瞬时吸收光谱（TAS）的晚期光谱技术将揭示CNX的光体物理学，并确定最严重的效率瓶颈。人们对光效率的能量，结构和空间异质性的影响很少了解。为了对确定光活性的关键过程进行整体视野，我的小组将研究在三个不同轴上修改的CNX的电荷载体动力学：（ NANO）形态，末端基团的化学性质和沉积的氧化还原cocatalysts。为了发现CNX中的空间异质性，我将开发微秒 - 第二个瞬态吸收显微镜（TAM），以绘制诸如电荷捕获，电荷累积和界面电荷转移等过程。光谱法将产生指导光催化剂的合成修饰所需的至关重要的辐射和结构见解。协同光谱和合成方法将优化有效的H2产生和CO2光元所需的CNX形态和内部光物理学。我的长期视力是利用优化的CNX光体物理学来开发太阳能驱动的碳捕获和利用，并使用CNX和光在具有较长寿命的材料中隔离CO2。 参与研究计划的HQP将获得合成，光谱，沟通和管理技能的独特组合，使它们对不断增长的清洁技术领域有吸引力。 HQP将为清洁能源领域和重要的H2行业做出贡献，该行业将在2025年底之前超过2000亿美元，发展加拿大的经济并帮助达到较低的CO2排放目标。