Electrolysis of water is widely used for hydrogen isotope separation and the development of hydrogen evolution reaction (HER) catalysts with high selectivity and activity is of key importance. Herein, we propose single atom catalysts (SACs) as promising catalysts for efficient hydrogen isotope separation. Pt SACs and Pt nanoparticles (NPs) have been fabricated on nanoarray-structured nitrogen-doped graphite foil (NGF) substrate by a polyol reduction method. The as prepared Pt1/NGF electrode exhibits high activity and selectivity toward HER with a low overpotential of 0.022 V at 10 mA·cm−2 and a high separation factor of 6.83 for hydrogen and deuterium separation, much better than Pt NPs counterpart. Density functional theory (DFT) calculations ascribe the high activity and selectivity to the constructed Pt-N2C2 structure. This work develops a new opportunity for the design and application of high-efficiency and stable SACs toward hydrogen isotope separation by electrolysis of water.
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Electrochemical coupling hydrogen evolution with biomass reforming reaction (named electrochemical hydrogen and chemical cogeneration (EHCC)), which realizes green hydrogen production and chemical upgrading simultaneously, is a promising method to build a carbon-neutral society. Herein, we analyze the EHCC process by considering the market assessment. The ethanol to acetic acid and hydrogen approach is the most feasible for large-scale hydrogen production. We develop AuCu nanocatalysts, which can selectively oxidize ethanol to acetic acid (> 97%) with high long-term activity. The isotopic and in-situ infrared experiments reveal that the promoted water dissociation step by alloying contributes to the enhanced activity of the partial oxidation reaction path. A flow-cell electrolyzer equipped with the AuCu anodic catalyst achieves the steady production of hydrogen and acetic acid simultaneously in both high selectivity (> 90%), demonstrating the potential scalable application for green hydrogen production with low energy consumption and high profitability.
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Green hydrogen has shown great potential to power microgrids as a primary source, whereas the resilient operation methodology under extreme events remains an open area. To fill this gap, this letter establishes an operational optimization strategy towards resilient hydrogen-powered microgrids. The frequency and voltage regulation characteristics of primary hydrogen sources under droop control and their electrical-chemical conversion process with nonlinear stack efficiency are accurately modeled by piecewise linear constraints. A resilience-oriented multi-time-slot stochastic optimization model is then formulated for an economic and robust operation under changing uncertainties. Test results show that the new formulation can leverage the primary hydrogen sources to achieve a resilience and safety-assured operation plan, supplying maximum critical loads while significantly reducing the frequency and voltage variations.
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Elasticity, as an emerging phenomenon of crystals, endows the newfangled properties on crystals owing to the altered local crystallinity in the deformed state, and hence attracts increasing research endeavors. However, only a few molecular crystals and a limited number of one-dimensional coordination polymer crystals have exhibited such fantastic elastic response under mechanical stress. Herein, we report the first example of elastic hydrogen-bonded ionic framework (HIF) of {(CN3H6)2[Ti(μ2-O)(SO4)2]}n, assembled from one-dimensional negatively charged inorganic [Ti(μ2-O)(SO4)2]n2n− chains and positively charged organic guanidinium cations via hydrogen bonds and electrostatic interactions. The slender prismatic single crystal exhibits remarkable elasticity with an optimal elastic bending strain (ε) of 2.5%. Impressively, the crystals give rise to two-dimensional elasticity owing to the equivalent crystallographic planes of the exposed faces and an unusual elastic response at liquid nitrogen temperature. The in-depth crystallographic analyses reveal hydrogen bonds and electrostatic interactions between anion chains and cations function like adhesive glue and account for such specific elastic properties, owing to the flexible and dynamic attributes of hydrogen bonds as they can work in a range of distance and orientation. And the channel in HIF provides space for bending with reduced strain. Incorporating these factors into low-dimensional crystals could be a general guidance for designing elastic crystals. Elasticity ganged with other intrinsic properties of HIF materials could inspire their newfangled applications in the near future.
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As a clean, efficient, and sustainable energy, hydrogen is expected to replace traditional fossil energy. A series of studies focusing on morphology regulation, surface modification, and structural reconstruction have been devoted to improving the intrinsic catalytic activity of non-noble metal catalysts. However, complex system structure design and the mutual interference of various chemical components would hinder the further improvement of hydrogen evolution performance. In recent years, external field assisted hydrogen evolution reaction (HER) has become a new research hotspot. Herein, we systematically summarize the promoting effects of various external fields on catalytic hydrogen production from the aspects of system design and catalytic mechanism, including electric field, thermal field, optical field, magnetic field, and acoustic field. Ultimately, we discuss the key challenges facing this external field regulation strategy and put forward the prospect of future research topics. We sincerely expect that this review could not only provide a new insight into the basic mechanism of external-assisted catalysis, but also promote further research on improving HER performance from a more diverse and comprehensive perspective.
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The diffusion, adsorption/desorption behaviors of water molecules and hydrogen molecules are of great importance in heterogeneous photocatalytic hydrogen production. In the study of structure–property–performance relationships, nanoconfined space provides an ideal platform to promote mass diffusion and transfer due to their extraordinary properties that are different from the bulk systems. Herein, we designed and prepared a nanoconfined CdS@SiO2-NH2 nanoreactor, whose shell is composed of amino-functionalized silica nanochannels, and encapsulates spherical CdS as a photocatalyst inside. Experimental and simulated results reveal that the amino-functionalized nanochannels promote water molecules’ and hydrogen molecules’ directional diffusion and transport. Water molecules are enriched in the nanocavity between the core and the shell, and promote the interfacial photocatalytic reaction. As a result, the maximized water enrichment and minimized hydrogen-occupied active sites enable photocatalyst with optimized mass transfer kinetics and localization electron distribution on the CdS surface, leading to superior hydrogen production performance with activity as high as 37.1 mmol·g−1·h−1.
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Direct CO2 hydrogenation offers an important strategy for promoting the global carbon balance, but high thermodynamic and kinetic stability of CO2 has restricted its applicability to only a handful of industrial sectors. Here, we introduce a proof-of-concept application of the electron-rich Pt surface to promote hydrogen donation for electron-rich MoC particles acting as hydrogen acceptors, thereby constructing hydrogen-rich surface of MoC active centers. Moreover, the formed hydrogen-rich and electron-rich surface could greatly decrease reaction activation energy to boost the efficient CO2 hydrogenation into formic acid over the MoC centers. The optimized MoC@NC/Pt-0.1 (NC: nitrogen-doped carbon) catalyst exhibits a high turnover frequency (TOF) value of 1.2 h−1 at a lower temperature of 60 °C and a TOF of 24.2 h−1 under standard reaction conditions widely used in the literature, exceeding 7 times of MoC@NC catalyst and surpassing the benchmark classical non-noble metal active center-based heterogeneous catalyst.
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Hydrogen detection with a high sensitivity is necessary for preventing potential explosions and fire. In this study, a novel ZnO tribotronic transistor is developed by coupling a ZnO field effect transistor (FET) and triboelectric nanogenerator in free-standing mode and is used as a sensor for hydrogen detection at room temperature. Tribotronic modulated performances of the hydrogen sensor are demonstrated by investigating its output characteristics at different sliding distances and hydrogen concentrations. By applying an external mechanical force to the device for sliding electrification, the detection sensitivity of the ZnO tribotronic transistor sensor is improved, with a significant enhancement achieved in output current by 62 times at 500 ppm hydrogen and 1 V bias voltage. This study demonstrates an extension of the applications of emerging tribotronics for gas detection and a prospective approach to improve the performance of the hydrogen sensor via human-interfacing.
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Hydrogen production from water electrolysis is a sustainable and environmentally benign strategy in comparison with fossil fuel-based hydrogen. However, this promising technique suffers from the high energy consumption and unsatisfactory cost due to the sluggish kinetics of both half reaction and inferior stability of electrocatalysts. To address this challenge, herein, we present a timely and comprehensive review on advances in alkaline water electrolysis that is already commercialized for large scale hydrogen production. The design principles and strategies with aiming to promote the performance of hydrogen generation are discussed from the view of electrocatalyst, electrode, reaction and system. The challenges and related prospects are presented at last, hopefully to provide essential ideas and to promote the wide application of hydrogen production.
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With the proposal of carbon neutrality goals and hydrogen energy development strategies in various countries, the development and construction of hydrogen supply chains have become important priorities. However, existing research has paid little attention to the hydrogen market and pricing. Therefore, a hydrogen pricing method based on marginal pricing theory is proposed in this paper, which adapts to hydrogen systems with renewable-to-hydrogen as a major source, in the future. A hydrogen energy market is established to define the industrial chain of hydrogen and the hydrogen trading process. The hydrogen market-clearing model is formulated considering a dynamic line pack. Due to its nonconvexity, the model is equivalently converted into mixed-integer second-order cone programming, and the optimality gap is minimized by introducing a penalty term. Based on the clearing solution, the concept and calculation method of the locational marginal hydrogen price (LMHP) are proposed with respect to the locational marginal price (LMP) in electricity markets. Case studies based on a modified Belgium 20-node gas network and Pennsylvania, New Jersey, and Maryland (PJM) market operation data demonstrate the consistency between LMHP and LMP.
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