More Like this

1. Visible-light-driven organic transformations integrated with H ₂ production on semiconductors

   https://doi.org/10.1039/D0MA00327A  

   Tang, Jian-Hong; Sun, Yujie (October 2020, Materials Advances)

   null (Ed.)

   Due to its clean and sustainable nature, solar energy has been widely recognized as a green energy source in driving a variety of reactions, ranging from small molecule activation and organic transformation to biomass valorization. Within this context, organic reactions coupled with H 2 evolution via semiconductor-based photocatalytic systems under visible light irradiation have gained increasing attention in recent years, which utilize both excited electrons and holes generated on semiconductors and produce two types of value-added products, organics and H 2 , simultaneously. Based on the nature of the organic reactions, in this review article we classify semiconductor-based photocatalytic organic transformations and H 2 evolution into three categories: (i) photocatalytic organic oxidation reactions coupled with H 2 production, including oxidative upgrading of alcohols and biomass-derived intermediate compounds; (ii) photocatalytic oxidative coupling reactions integrated with H 2 generation, such as C–C, C–N, and S–S coupling reactions; and (iii) photo-reforming reactions together with H 2 formation using organic plastics, pollutants, and biomass as the substrates. Representative heterogeneous photocatalytic systems will be highlighted. Specific emphasis will be placed on their synthesis, characterization, and photocatalytic mechanism, as well as the organic reaction scope and practical application. 

   more » « less
2. Integrated design for electrocatalytic carbon dioxide reduction

   https://doi.org/10.1039/D0CY00453G  

   Zhao, Xin; Du, Lijie; You, Bo; Sun, Yujie (May 2020, Catalysis Science & Technology)

   null (Ed.)

   The electrocatalytic carbon dioxide reduction reaction (CO 2 RR) to produce valuable fuels and chemicals with renewable energy inputs is an attractive route to convert intermittent green energy sources ( e.g. , solar and wind) to chemical energy, alleviate our dependence on fossil fuels, and simultaneously reduce net carbon dioxide emission. However, the generation of reduced multi-carbon products with high energy density and wide applicability from the CO 2 RR, such as oxygenates and hydrocarbons, suffers from high overpotential, slow reaction rate, and low selectivity due to its intrinsic multi-electron transfer nature. Moreover, the involved anodic oxygen evolution reaction (OER) also requires large overpotential and its product O 2 bears limited economic value. The potentially generated reactive oxygen species (ROS) during the OER may also degrade the membrane of a CO 2 reduction electrolyzer. Herein, we review the recent progress in novel integrated strategies to address the aforementioned challenges in the electrocatalytic CO 2 RR. These innovative strategies include (1) concurrent CO 2 electroreduction via co-feeding additional chemicals besides CO 2 gas, (2) tandem CO 2 electroreduction utilizing other catalysts for converting the in situ formed products from the CO 2 RR into more valuable chemicals, and (3) hybrid CO 2 electroreduction through integrating thermodynamically more favourable organic upgrading reactions to replace the anodic OER. We specifically highlight these novel integrated electrolyzer designs instead of focusing on nanostructured engineering of various electrocatalysts, in the hope of inspiring others to approach CO 2 electroreduction from a holistic perspective. The current challenges and future opportunities of electrocatalytic CO 2 reduction will also be discussed at the end. 

   more » « less
3. Lead halide perovskites for photocatalytic organic synthesis

   https://doi.org/10.1038/s41467-019-10634-x  

   Zhu, Xiaolin; Lin, Yixiong; San Martin, Jovan; Sun, Yue; Zhu, Dian; Yan, Yong (June 2019, Nature Communications)

   Abstract Nature is capable of storing solar energy in chemical bonds via photosynthesis through a series of C–C, C–O and C–N bond-forming reactions starting from CO₂and light. Direct capture of solar energy for organic synthesis is a promising approach. Lead (Pb)-halide perovskite solar cells reach 24.2% power conversion efficiency, rendering perovskite a unique type material for solar energy capture. We argue that photophysical properties of perovskites already proved for photovoltaics, also should be of interest in photoredox organic synthesis. Because the key aspects of these two applications are both relying on charge separation and transfer. Here we demonstrated that perovskites nanocrystals are exceptional candidates as photocatalysts for fundamental organic reactions, for example C–C, C–N and C–O bond-formations. Stability of CsPbBr₃in organic solvents and ease-of-tuning their bandedges garner perovskite a wider scope of organic substrate activations. Our low-cost, easy-to-process, highly-efficient, air-tolerant and bandedge-tunable perovskites may bring new breakthrough in organic chemistry. 

   more » « less
4. Designing Simple Conjugated Polymers for Scalable and Efficient Organic Solar Cells

   https://doi.org/10.1002/cssc.202100910  

   Rech, Jeromy_James; Neu, Justin; Qin, Yunpeng; Samson, Stephanie; Shanahan, Jordan; Josey, III, Richard_F; Ade, Harald; You, Wei (June 2021, ChemSusChem)

   Abstract Conjugated polymers have a long history of exploration and use in organic solar cells, and over the last twenty‐five years, marked increases in the solar cell efficiency have been achieved. However, the synthetic complexity of these materials has also drastically increased, which makes the scalability of the highest‐efficiency materials difficult. If conjugated polymers could be designed to exhibit both high efficiency and straightforward synthesis, the road to commercial reality would be more achievable. For that reason, a new synthetic approach was designed towards PTQ10 (=poly[(thiophene)‐alt‐(6,7‐difluoro‐2‐(2‐hexyldecyloxy)quinoxaline)]). The new synthetic approach to make PTQ10 brought a significant reduction in cost (1/7th the original) and could also easily accommodate different side chains to move towards green processing solvents. Furthermore, high‐efficiency organic solar cells were demonstrated with a PTQ10:Y6 blend exhibiting approximately 15 % efficiency. 

   more » « less
5. Photoelectrochemical water splitting under concentrated sunlight: best practices and protocols

   https://doi.org/10.3389/fenrg.2025.1550153  

   Li, Kejian; Dong, Wan Jae; Mi, Zetian (March 2025, Frontiers in Energy Research)

   Photoelectrochemical (PEC) water splitting is a promising technology for green hydrogen production by harnessing solar energy. Traditionally, this sustainable approach is studied under light intensity of 100 mW/cm²mimicking the natural solar irradiation at the Earth’s surface. Sunlight can be easily concentrated using simple optical systems like Fresnel lens to enhance charge carrier generation and hydrogen production in PEC water splitting. Despite the great potentials, this strategy has not been extensively studied and faces challenges related to the stability of photoelectrodes. To prompt the investigations and applications, this work outlines the best practices and protocols for conducting PEC solar water splitting under concentrated sunlight illumination, incorporating our recent advancements and providing some experimental guidelines. The key factors such as light source calibration, photoelectrode preparation, PEC cell configuration, and long-term stability test are discussed to ensure reproducible and high performance. Additionally, the challenges of the expected photothermal effect and the heat energy utilization strategy are discussed. 

   more » « less