• Energy Research

The development of efficient catalysts for the direct synthesis of higher alcohols (HA) via CO hydrogenation has remained a prominent research challenge. While modified Fischer-Tropsch synthesis (m-FTS) systems hold great potential, they often retain limited active site density under operating conditions for industrially relevant performance. Aimed at improving existing catalyst architectures, this study investigates the impact of highly dispersed metal oxides of Co-Cu, Cu-Fe, and Co-Fe m-FTS systems and demonstrates the viability of ZrO2 as a general promoter in the direct synthesis of HA from syngas. A volcano-like composition-performance relationship, in which 5-10 mol % ZrO2 resulted in maximal HA productivity, governs all catalyst families. The promotional effect resulted in a 2.5-fold increase in HA productivity for the optimized Cu1Co4@ZrO2-5 catalyst (Cu:Co = 1:4, 5 mol % ZrO2) compared to its ZrO2-free counterpart and placed Co1Fe4@ZrO2-10 among the most productive systems (345 mgHA h-1 gcat-1) reported in this category under comparable operating conditions, with stable performance for at least 300 h. ZrO2 assumes an amorphous and defective nature on the catalysts, leading to enhanced H2 and CO activation, facilitated formation of metallic and carbide phases, and structural stabilization.

We analyse the future transition towards a carbon-neutral chemical sector. Our study unfolds new avenues to include SDG-based metrics in science and engineering while quantifying the potential collateral damage of CCU on sustainable development.

AbstractMethanol production with the use of syngas derived from solar‐driven splitting of CO2 and H2O is a promising route to sustainable liquid fuels. Herein, we investigated the effect of using a CO2‐rich syngas with the same composition as that obtained in a solar thermochemical reactor and of applying a daily startup–shutdown (DSS) routine matching the intermittent solar operation over a benchmark Cu–ZnO–Al2O3 catalyst. The catalyst reached fast equilibration (10 h) in the presence of this syngas mixture and reversibly responded to changes in the concentrations of CO and CO2 by mimicking fluctuations in the feed composition. Remarkably, its deactivation was even less pronounced over 27 cycles under a DSS regime than for a corresponding time on stream under uninterrupted operation if the reactor was purged with H2‐free syngas upon shutdown. Characterization and modeling indicated that this purging avoided the formation of inactive ZnCO3 and minimized the oxidation of the Cu surface atoms.

Wax on, wax off: Bifunctional cobalt-based catalysts on zeolite supports are applied for the valorization of biosyngas through Fischer-Tropsch chemistry. By using these catalysts, waxes can be hydrocracked to shorter-chain hydrocarbons, increasing the selectivity towards the C5 -C11 (gasoline) fraction. The zeolite topology and the amount and strength of acid sites are key parameters to maximize the performance of these bifunctional catalysts, steering Fischer-Tropsch product selectivity towards liquid hydrocarbons.

We quantify the absolute environmental sustainability of DME-fuelled heavy-duty (HD) trucks, and compare it against the current diesel counterpart, finding that renewable DME can promote an absolute environmentally sustainable HD truck sector.

Dataset supporting the article "Assessing the environmental benefit of palladium-based single-atom heterogeneous catalysts for Sonogashira coupling" by D. Faust Akl, D. Poier, S. C. D’Angelo, T. P. Araújo, V. Tulus, O. V. Safonova, S. Mitchell, R. Marti, G. Guillén-Gosálbez, and J. Pérez-Ramírez.

At present, the synthesis of ammonia through the Haber-Bosch (HB) process accounts for 1.2% of the global carbon emissions, representing roughly one-fourth of the global fossil consumption from the chemical industry, which creates a pressing need for alternative low-carbon synthesis routes. Analyzing seven essential planetary boundaries (PBs) for the safe operation of our planet, we find that the standard HB process is unsustainable as it vastly transgresses the climate change PB. In order to identify more responsible strategies from this integrated perspective, we assess the absolute sustainability level of 34 alternative routes where hydrogen (H-2) is supplied by steam methane reforming with carbon capture and storage, biomass gasification, or water electrolysis powered by various energy sources. We found that some of these scenarios could substantially reduce the global impact of fossil HB, yet alleviating the impact on climate change could critically exacerbate the impacts on other Earth-system processes. Furthermore, we identify that reducing the cost of electrolytic H-2 is the main avenue toward the economic appeal of the most sustainable routes. Our work highlights the need to embrace global impacts beyond climate change in the assessment of decarbonization routes of fossil chemicals. This approach enabled us to identify more suitable alternatives and associated challenges toward environmental and economically attractive ammonia synthesis. ACS Sustainable Chemistry & Engineering, 9 (29) ISSN:2168-0485

A major challenge for achieving the energy transition and transforming the current energy model into distributed production is the development of efficient artificial leaf devices made of earth-abundant materials for sustainable fuel production.