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Developing atomically synergistic bifunctional catalysts relies on the creation of colocalized active atoms to facilitate distinct elementary steps in catalytic cycles. Herein, we show that the atomically-synergistic binuclear-site catalyst (ABC) consisting of [Formula: see text]-O-Cr6+ on zeolite SSZ-13 displays unique catalytic properties for iso-stoichiometric co-conversion of ethane and CO2. Ethylene selectivity and utilization of converted CO2 can reach 100 % and 99.0% under 500  °C at ethane conversion of 9.6%, respectively. In-situ/ex-situ spectroscopic studies and DFT calculations reveal atomic synergies between acidic Zn and redox Cr sites. [Formula: see text] ([Formula: see text]) sites facilitate β-C-H bond cleavage in ethane and the formation of Zn-Hδ- hydride, thereby the enhanced basicity promotes CO2 adsorption/activation and prevents ethane C-C bond scission. The redox Cr site accelerates CO2 dissociation by replenishing lattice oxygen and facilitates H2O formation/desorption. This study presents the advantages of the ABC concept, paving the way for the rational design of novel advanced catalysts.

The over 15 million metric tonnes of carbon black produced annually emit carbon dioxide in the range of 29–79 million metric tonnes each year. With the renaissance of carbon black in many new renewable energy applications as well as the growing transportation sector, where carbon black is used as a rubber reinforcement agent in car tires, the carbon black market is expected to grow by 66% over the next 9 years. As such, it is important to better understand energy intensity and carbon dioxide emissions of carbon black production. In this work, the furnace black process is studied in detail using process models to provide insights into mass and energy balances, economics, and potential pathways for lowering the environmental impact of carbon black production. Current state-of-the-art carbon black facilities typically flare the tail gas of the carbon black reactor. While low in heating value, this tail gas contains considerable amounts of energy and flaring this tail gas leads to low overall efficiency (39.6%). The efficiency of the furnace black process can be improved if the tail gas is used to produce electricity. However, the high capital investment cost and increased operating costs make it difficult to operate electricity generation from the tail gas economically. Steam co-generation (together with electricity generation) on the other hand is shown to substantially improve energy efficiency as well as economics, provided that steam users are nearby. Steam co-generation can be achieved via back-pressure steam turbines so that the low-pressure exhaust steam (∼2 bar/120 °C) can be used locally for heating or drying purposes. Furthermore, the potential of utilizing hydrogen to reduce carbon dioxide emissions is investigated. Using hydrogen as fuel for the carbon black reactor instead of natural gas is shown to reduce the carbon dioxide footprint by 19%. However, current prices of hydrogen lead to a steep increase in the levelized cost of carbon black (47%).

Solid oxide fuel cell (SOFC)–gas turbine (GT) hybrid systems can produce power at high electrical efficiencies while emitting virtually zero criteria pollutants (e.g., ozone, carbon monoxide, oxides of nitrogen and sulfur, and particulate matters). This study presents new insights into renewable hydrogen (RH2)-powered SOFC–GT hybrid systems with respect to their system configuration and techno-economic analysis motivated by the need for clean on-demand power. First, three system configurations are thermodynamically assessed: (I) a reference case with no SOFC off-gas recirculation, (II) a case with cathode off-gas recirculation, and (III) a case with anode off-gas recirculation. While these configurations have been studied in isolation, here we provide a detailed performance comparison. Moreover, a techno-economic analysis is conducted to study the economic competitiveness of RH2-fueled hybrid systems and the economies of scale by offering a comparison to natural gas (NG)-fueled systems. Results show that the case with anode off-gas recirculation, with 68.50%-lower heating value (LHV) at a 10 MW scale, has the highest efficiency among the studied scenarios. When moving from 10 MW to 50 MW, the efficiency increases to 70.22%-LHV. These high efficiency values make SOFC–GT hybrid systems highly attractive in the context of a circular economy as they outcompete most other power generation technologies. The cost-of-electricity (COE) is reduced by about 10% when moving from 10 MW to 50 MW, from USD 1976/kW to USD 1668/kW, respectively. Renewable H2 is expected to be economically competitive with NG by 2030, when the U.S. Department of Energy’s target of USD 1/kg RH2 is reached.

Hydrogen-based direct reduced iron (H2-DRI) is an alternative pathway for low-carbon steel production. Yet, the lack of established process and business models defining “green steel” makes it difficult to understand what the respective H2 price has to be in order to be competitive with commercial state-of-the-art natural gas DRI. Given the importance of establishing break-even H2 prices and CO2 emission reduction potentials of H2-DRI, this study conducted techno-economic analyses of several design and operation scenarios for DRI systems. Results show that renewable H2 use in integrated DRI steel mills for both heating and the reduction of iron ore can reduce direct CO2 emissions by as much as 85%, but would require an H2 procurement cost of $1.63 per kg H2 or less. When using H2 only for iron ore reduction, economic viability is reached at an H2 procurement cost of $1.70 per kg, while achieving a CO2 emission reduction of 76% at the plant site. System design optimization strategies around excess H2 ratios in the DRI top gas and the H2 recycle pressurization can further improve performance and economics. Low H2 excess ratios are particularly attractive as they reduce pre-heating energy requirements and offer integration opportunities with static recycle ejectors if H2 is supplied at sufficiently high pressure. The potential of utilizing the electric arc furnace off-gas is shown to be much more synergistic with H2-DRI than natural gas-DRI and can increase the break-even H2 procurement cost by up to 7¢ per kg H2. Such findings are critical for setting technical performance criteria for H2 supply and storage in the iron and steel sector.

Electrochemical oxidative coupling of methane (E-OCM) with Sr2Fe1·5Mo0·5O6−δ (SFM) catalyst is demonstrated with metal-supported solid oxide cells (MS-SOC). SFM anode and Pr6O11 cathode catalysts are loaded into a porous symmetric-architecture cell by infiltration and firing. The most effective chelating agent (citric acid/ethyl glycol) and optimal firing/reducing temperatures (850 °C/750 °C) for the SFM catalyst precursor solution are selected and confirmed by cell testing. Operating temperature, cell voltage, and oxygen concentration at the cathode greatly affect the methane conversion rate and product selectivity by controlling the oxygen ion flow. CH4 conversion of 85.8% is obtained, with C2H4, C2H6, and H2 concentrations of 10.5%, 12.3%, and 25.6% at 800 °C, respectively, in the product exhaust gas. Reasonable stability of the current density and methane conversion is demonstrated during 200 h operation. This research demonstrates technical progress in catalyst and device development for the E-OCM reaction to synthesize valuable chemicals.

Substantial upscaling of carbon dioxide capture is possible in the coming decades but existing solutions for storage are projected to be limited in annual capacity by as much as 2-10 GtCO2 per year until mid-century. Temporary storage of CO2 in a solid or liquid state could prove useful for filling this gap in capacity, until more permanent and ideally lucrative CO2 sequestration options come online. There are several concepts for reversible solid-state and chemical CO2 storage, but their advantages and limitations have yet to be reviewed in this context. This article focuses on the physical and chemical aspects of CO2 storage via liquid and solid chemical carriers and sorbents, and gives an overview of the energetics around their use, as well as prospects for their future development. Exciting opportunities for coupling capture and medium to high maturity multi-year storage technologies could support carbon removal in the coming decades. Highlights of the analysis are the remarkable storage capacity of oxalic acid and formic acid (CO2-density of 1857 kg m−3 and 1152 kg m−3, compared with condensed liquid CO2 at 993-1096 kg m−3, respectively), the relative scalability and compatibility of carbonate salts for stationary storage with direct air capture, and the potential promise of multiple carriers for CO2 transportation. Solid sorbents do not achieve such ultra-high storage capacities, but could improve storage over compressed gas tanks on a capacity and energetics basis.

The maximum firing temperature of a gas turbine (GT) is limited by material constraints. Critical for the operation of the GT is the blade metal temperature, which is impacted by the heat transfer from the combustor outlet gas to the blade surface. In this study, performance characteristics for an H-class-type GT have been established and two correlations for the change in the maximum permissible firing temperature as function of combustor outlet gas composition or flue gas composition and pressure ratio have been derived: (I) for detailed GT modeling with cooling flows and (II) for simplified GT modeling without specifying cooling flows. [ABSTRACT FROM AUTHOR]

Steady state simulations were carried out in APSEN Plus®, state-point stream data were extracted from the simulation results and tabulated in sequential order for IGCC configurations. These data give detailed insights into the performance of individual process units and enable researches to better understand the interplay of various process units as well as provide data for reproducibility of the work described in Ref. (Rosner et al., 2019). Furthermore, more detailed insights in the economic analysis are garnered by providing itemized capital and operating cost data as well as the individual unit cost correlations. In addition, a detailed plant water balance is provided for the base cases of the cold gas cleanup scenario and warm gas cleanup scenario., (© 2019 The Author(s).)