2021, Liu, Yannan, Chen, Chuanshuang, Valdez, Jesus, Meira, Debora Motta, He, Wanting, Wang, Yong, Harnagea, Catalin, Lu, Qiongquiong, Guner, Tugrul, Wang, Hao, Liu, Cheng-Hao, Zhang, Qingzhe, Huang, Shengyun, Yurtsever, Aycan, Chaker, Mohamed, Ma, Dongling

Conversion of clean solar energy to chemical fuels is one of the promising and up-and-coming applications of metal–organic frameworks. However, fast recombination of photogenerated charge carriers in these frameworks remains the most significant limitation for their photocatalytic application. Although the construction of homojunctions is a promising solution, it remains very challenging to synthesize them. Herein, we report a well-defined hierarchical homojunction based on metal–organic frameworks via a facile one-pot synthesis route directed by hollow transition metal nanoparticles. The homojunction is enabled by two concentric stacked nanoplates with slightly different crystal phases. The enhanced charge separation in the homojunction was visualized by in-situ surface photovoltage microscopy. Moreover, the as-prepared nanostacks displayed a visible-light-driven carbon dioxide reduction with very high carbon monooxide selectivity, and excellent stability. Our work provides a powerful platform to synthesize capable metal–organic framework complexes and sheds light on the hierarchical structure-function relationships of metal–organic frameworks.

2018, Wohland, Jan, Witthaut, Dirk, Schleussner, Carl-Friedrich

The mitigation of climate change requires fast reductions in greenhouse gas emissions and calls for fundamental transitions of energy systems. In most places, the increased exploitation of variable renewable sources (wind and solar) forms the backbone of these transitions. To remain consistent with the Paris Agreement temperature goals, negative emission technologies will likely be needed to achieve net zero emissions in the second half of the century. In integrated assessment models, negative emissions are typically realized through land-based approaches. However, due to their coarse temporal and spatial resolution, such models might underestimate the potential of decentrally deployable and flexible technologies such as Direct Air Capture (DAC). Based on validated high-resolution power generation time series, we show that DAC can extract CO2 from the atmosphere and facilitate the integration of variable renewables at the same time. It is a promising flexibility provider as it can be ramped within minutes. Our results show that negative emissions of up to 500 Mt CO2/year in Europe may be achievable by using renewable excess energy only. Electricity systems with high shares of volatile renewables will induce excess generation events during which electricity is cheap thereby lowering the operational costs of DAC. If investment costs can be sufficiently reduced, this may render very energy intensive but highly flexible technologies such as DAC viable.