2.3. Evaluation of Photocatalytic Water Splitting 6507 2.3.1. Photocatalytic Activity 6507 2.3.2. Photocatalytic Stability 6507 3. UV-Active Photocatalysts for Water Splitting 6507 3.1. d0 Metal Oxide Photocatalyts 6507 3.1.1. Ti-, Zr-Based Oxides 6507 3.1.2. Nb-, Ta-Based Oxides 6514 3.1.3. W-, Mo-Based Oxides 6517 3.1.4. Other d0 Metal Oxides 6518 3.2. d10 Metal Oxide Photocatalyts 6518 3.3. f0 Metal Oxide Photocatalysts 6518 3.4. Nonoxide Photocatalysts 6518 4. Approaches to Modifying the Electronic Band Structure for Visible-Light Harvesting 6519

Semiconductor-based Photocatalytic Hydrogen Generation

Generations Yi Ma,† Xiuli Wang,† Yushuai Jia,† Xiaobo Chen,‡ Hongxian Han,*,† and Can Li*,† †State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences and Dalian National Laboratory for Clean Energy, 457 Zhongshan Road, Dalian 116023, China ‡Department of Chemistry, College of Arts and Sciences, University of Missouri-Kansas City, 5100 Rockhill Road, Kansas City, Missouri 64110, United States

Titanium dioxide-based nanomaterials for photocatalytic fuel generations.

Solar-driven water splitting provides a leading approach to store the abundant yet intermittent solar energy and produce hydrogen as a clean and sustainable energy carrier. A straightforward route to light-driven water splitting is to apply self-supported particulate photocatalysts, which is expected to allow solar hydrogen to be competitive with fossil-fuel-derived hydrogen on a levelized cost basis. More importantly, the powder-based systems can lend themselves to making functional panels on a large scale while retaining the intrinsic activity of the photocatalyst. However, all attempts to generate hydrogen via powder-based solar water-splitting systems to date have unfortunately fallen short of the efficiency values required for practical applications. Photocatalysis on photocatalyst particles involves three sequential steps: (i) absorption of photons with higher energies than the bandgap of the photocatalysts, leading to the excitation of electron-hole pairs in the particles, (ii) charge separation and migration of these photoexcited carriers, and (iii) surface chemical reactions based on these carriers. In this review, we focus on the challenges of each step and summarize material design strategies to overcome the obstacles and limitations. This review illustrates that it is possible to employ the fundamental principles underlying photosynthesis and the tools of chemical and materials science to design and prepare photocatalysts for overall water splitting.

Particulate Photocatalysts for Light-Driven Water Splitting: Mechanisms, Challenges, and Design Strategies

Hydrogen from solar-driven water splitting has the potential to provide clean energy. Current progress towards artificial photosynthetic devices is reviewed, with particular focus on visible light active nanostructures. A vision for a future sustainable hydrogen fuel community based on artificial photosynthesis is outlined.

Artificial photosynthesis for solar water-splitting

There is a growing interest in the conversion of water and solar energy into clean and renewable H2 fuels using earth-abundant materials due to the depletion of fossil fuel and its serious environmental impact. This critical review highlights some key factors influencing the efficiency of heterogeneous semiconductors for solar water splitting (i.e. improved charge separation and transfer, promoted optical absorption, optimized band gap position, lowered cost and toxicity, and enhanced stability and water splitting kinetics). Moreover, different engineering strategies, such as band structure engineering, micro/nano engineering, bionic engineering, co-catalyst engineering, surface/interface engineering of heterogeneous semiconductors are summarized and discussed thoroughly. The synergistic effects of the different engineering strategies, especially for the combination of co-catalyst loading and other strategies seem to be more promising for the development of highly efficient photocatalysts. A thorough understanding of electron and hole transfer thermodynamics and kinetics at the fundamental level is also important for elucidating the key efficiency-limiting step and designing highly efficient solar-to-fuel conversion systems. In this review, we provide not only a summary of the recent progress in the different engineering strategies of heterogeneous semiconductors for solar water splitting, but also some potential opportunities for designing and optimizing solar cells, photocatalysts for the reduction of CO2 and pollutant degradation, and electrocatalysts for water splitting.

Engineering heterogeneous semiconductors for solar water splitting

A study of hybrid, enzyme-modified nanoparticles able to produce H2 using visible light as the energy source has been carried out to establish per-site performance standards for H2 production catalysts able to operate under ambient conditions. The [NiFeSe]-hydrogenase from Desulfomicrobium baculatum (Db [NiFeSe]-H) is identified as a particularly proficient catalyst. The optimized system consisting of Db [NiFeSe]-H attached to Ru dye-sensitized TiO2, with triethanolamine as a sacrificial electron donor, produces H2 at a turnover frequency of approximately 50 (mol H2) s−1 (mol total hydrogenase)−1 at pH 7 and 25 °C, even under the typical solar irradiation of a northern European sky. The system shows high electrocatalytic stability not only under anaerobic conditions but also after prolonged exposure to air, thus making it sufficiently robust for benchtop applications.

Visible Light-Driven H2 Production by Hydrogenases Attached to Dye-Sensitized TiO2 Nanoparticles

Changes in ambient temperature affect all biological processes. However, these effects are process specific and often vary non-linearly. It is thus a non-trivial problem for neuronal circuits to maintain coordinated, functional output across a range of temperatures. The cardiac nervous systems in two species of decapod crustaceans, Homarus americanus and Cancer borealis, can maintain function across a wide but physiologically relevant temperature range. However, the processes that underlie temperature resilience in neuronal circuits and muscle systems are not fully understood. Here, we demonstrate that the non-isolated cardiac nervous system (i.e., the whole heart: neurons, effector organs, intrinsic feedback systems) in the American lobster, H. americanus, is more sensitive to warm temperatures than the isolated cardiac ganglion (CG) that controls the heartbeat. This was surprising as modulatory processes known to stabilize the output from the CG are absent when the ganglion is isolated. One source of inhibitory feedback in the intact cardiac neuromuscular system is nitric oxide (NO), which is released in response to heart contractions. We hypothesized that the greater temperature tolerance observed in the isolated CG is due to the absence of NO feedback. Here, we demonstrate that applying an NO donor to the isolated CG reduces its temperature tolerance. Similarly, we show that the NO synthase inhibitor L-nitroarginine (LNA) increases the temperature tolerance of the non-isolated nervous system. This is sufficient to explain differences in temperature tolerance between the isolated CG and the whole heart. However, in an intact lobster, the heart and CG are modulated by an array of endogenous peptides and hormones, many of which are positive regulators of the heartbeat. Many studies have demonstrated that excitatory modulators increase temperature resilience. However, this neuromuscular system is regulated by both excitatory and inhibitory peptide modulators. Perfusing SGRNFLRFamide, a FLRFamide-like peptide, through the heart increases the non-isolated nervous system’s tolerance to high temperatures. In contrast, perfusing myosuppressin, a peptide that negatively regulates the heartbeat frequency, decreases the temperature tolerance. Our data suggest that, in this nervous system, positive regulators of neural output increase temperature tolerance of the neuromuscular system, while modulators that decrease neural output decrease temperature tolerance.

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The role of feedback and modulation in determining temperature resiliency in the lobster cardiac nervous system

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Visible Light-Driven H2 Production by Hydrogenases Attached to Dye-Sensitized TiO2 Nanoparticles

The role of feedback and modulation in determining temperature resiliency in the lobster cardiac nervous system