Syngas Selectivity Research Articles

Synergistic plasma and platinum catalysts interactions in CO2 reforming of propane at room temperature: The role of supports

This study investigates the synergistic impact of plasma and catalyst in a hybrid non-thermal plasma system integrated with 1 wt% Pt catalysts supported on diverse catalyst supports (γ-Al2O3, SBA-15, HZSM-5, CeO2, TiO2, and multi-wall carbon nanotube (CNT)) at ambient conditions in dry reforming of propane (DRP). To optimize the reaction, the impact of in-situ plasma reduction time was investigated over the Pt/Al2O3 catalyst at varying durations before the DRP reaction. The most favorable catalytic performance was observed at a reduction time of 60 min due to having the highest surface area (284 m2/g), which might result in smaller Pt particle size, and the effective reduction of oxidation states to Pt0. A comparison of reduction sources also revealed that the plasma-reduced catalyst outperformed the other, which was attributed to the agglomeration of Pt active sites during the thermal reduction process. The chemo-physical properties of different catalysts directly affected the plasma characteristics and catalytic performance. Pt/Al2O3 exhibited the highest performance, attributed to having the smallest mean Pt particle size (0.94 nm) and highest discharge power (13.97 W), effective capacitance (1.41 nF), and charge transfer (0.34 μC) during DRP reaction, leading to a 13 % and 15 % increase in CO2 and C3H8 conversions, respectively, compared to plasma-only mode. The catalytic performance showed that the synergy of catalysts with higher basic sites and plasma characteristics, along with smaller Pt particle size, resulted in high reactant conversion and syngas selectivity. Binary HRTEM images also indicated the presence of more soft carbon (coke) in the pore channels of the spent Pt/HZSM-5 catalyst than in spent Pt/Al2O3.

Fe–Ni composite oxygen carrier for chemical looping gasification with diverse fuels to produce syngas

Coal-based chemical looping gasification (CCLG) has been proposed as an emergent type of coal gasification technology that produces high-quality syngas by using lattice oxygen from oxygen carrier instead of molecular oxygen. In this paper, the Fe–Ni composite oxygen carrier was synthetized using sol-gel method and the gasification performance of the prepared sample was analyzed by a fixed-bed reactor. The results indicated that the Fe–Ni composite oxygen carrier presented a high carbon conversion of fuel and syngas selectivity during the CCLG process. Additionally, the cycle stability test showed that the carbon conversion of fuel and syngas selectivity did not change significantly with the increase of cyclic frequency. To further study the influence of volatiles released from coal on the gasification performance of oxygen carrier, the interactions between the oxygen carrier samples and char obtained at different pyrolysis temperatures were investigated by a fixed-bed reactor and TG-MS, respectively. The results suggested that the gas products (H2, CO, CO2 and CH4) yields of char-oxygen carrier were significantly lower than those of coal-oxygen carrier. Besides, the pyrolysis temperature for preparing char had a great effect on the carbon conversion of fuel and syngas selectivity due to the distinction of volatiles released from solid fuel.

Subsurface A-site vacancy activates lattice oxygen in perovskite ferrites for methane anaerobic oxidation to syngas

Tuning the oxygen activity in perovskite oxides (ABO3) is promising to surmount the trade-off between activity and selectivity in redox reactions. However, this remains challenging due to the limited understanding in its activation mechanism. Herein, we propose the discovery that generating subsurface A-site cation (Lasub.) vacancy beneath surface Fe-O layer greatly improved the oxygen activity in LaFeO3, rendering enhanced methane conversion that is 2.9-fold higher than stoichiometric LaFeO3 while maintaining high syngas selectivity of 98% in anaerobic oxidation. Experimental and theoretical studies reveal that absence of Lasub.-O interaction lowered the electron density over oxygen and improved the oxygen mobility, which reduced the barrier for C-H bond cleavage and promoted the oxidation of C-atom, substantially boosting methane-to-syngas conversion. This discovery highlights the importance of A-site cations in modulating electronic state of oxygen, which is fundamentally different from the traditional scheme that mainly credits the redox activity to B-site cations and can pave a new avenue for designing prospective redox catalysts.

Atomically dispersed MoNi alloy catalyst for partial oxidation of methane

The catalytic partial oxidation of methane (POM) presents a promising technology for synthesizing syngas. However, it faces severe over-oxidation over catalyst surface. Attempts to modify metal surfaces by incorporating a secondary metal towards C–H bond activation of CH4 with moderate O* adsorption have remained the subject of intense research yet challenging. Herein, we report that high catalytic performance for POM can be achieved by the regulation of O* occupation in the atomically dispersed (AD) MoNi alloy, with over 95% CH4 conversion and 97% syngas selectivity at 800 °C. The combination of ex-situ/in-situ characterizations, kinetic analysis and DFT (density functional theory) calculations reveal that Mo-Ni dual sites in AD MoNi alloy afford the declined O2 poisoning on Ni sites with rarely weaken CH4 activation for partial oxidation pathway following the combustion reforming reaction (CRR) mechanism. These results underscore the effectiveness of CH4 turnovers by the design of atomically dispersed alloys with tunable O* adsorption.

Enhanced reactivity over Ce2(SO4)3/MgO with NiO modification for chemical looping partial oxidation of methane

Chemical looping partial oxidation of methane to syngas is a promising process. Thermodynamic and kinetic analysis both forecast the NiO/Ce2(SO4)3–MgO is a prospective oxygen carrier (OC) to this process, which enables with 100% syngas selectivity, 2.15H2/CO ratio, excellent methane conversion and stable cycling characteristic. Compared with Ce2(SO4)3, the methane conversion rate rise by 73.19% because of the excellent lattice oxygen availability, less carbon deposit, and large specific surface area. The distinctive pore structure also provides a favorable reaction environment. Through the density functional theory, Ni doping can lower the energy barrier (Eb), promote lattice oxygen activation and diffusion, and the oxygen vacancy (Ov) can further promote these processes. CH3 → CH2 + H (TS2) is the rate-limiting step. Compared with Ce2(SO4)3, the Ni doping can reduce Eb by 16.8%, and the Ov can further reduce it by 43.0%. It does not change when the Ov concentration is more than 1.96%.

Halite-structured (MgCoNiMnFe)Ox high entropy oxide (HEO) for chemical looping dry reforming of methane

The configurational disorder of high entropy oxides (HEOs) promotes the reversible exsolution–redissolution of constituent metal species. This unique feature could be exploited to facilitate cyclic lattice oxygen storage and exchange. Herein, we report an in situ generated, halite-structured (MgCoNiMnFe)Ox HEO, which simultaneously functions as a redox catalyst and an oxygen carrier for dry reforming of methane in a chemical looping process (CL–DRM). Accordingly, the (MgCoNiMnFe)Ox/ZrO2 HEO catalyst exhibits outstanding DRM activity, syngas selectivity and cyclic stability compared to medium-entropy oxides and bimetallic oxides over 100 CL–DRM cycles at 800 °C. XRD analysis verified the entropy-mediated preservation of the alloy/HEO/ZrO2 catalytic structure over CL–DRM cycles. XAFS studies revealed the reversible and cyclic evolution–dissolution of Ni, Fe, Co over redox cycles. The exsolved NiFeCo nanoalloy exhibited high efficiency in activating CH4. This study has demonstrated the potential applications of HEO-based catalysts in efficient chemical looping processes.

Advances and Challenges in Oxygen Carriers for Chemical Looping Partial Oxidation of Methane

To cope with global warming and increasing carbon emissions, the chemical looping process has attracted attention due to its excellent ability to convert fossil fuel and capture CO2. In this case, chemical looping partial oxidation technology has become the focus of attention due to its advantages in the production of syngas and hydrogen, especially with respect to the design and selection of oxygen carriers, which directly affect the efficiency of the production of syngas and hydrogen. In particular, the conversion of methane can reach 95% in the chemical looping partial oxidation of methane, and the selectivity of syngas, in the range of 700 °C to 900 °C at atmospheric pressure, can reach 99% for twenty or more cycles. In this review, from the perspective of metal oxide selection and structure regarding the chemical looping partial oxidation process, we discuss the role of oxygen carriers in the chemical looping partial oxidation cycle, in which the specific surface area, the lattice oxygen mobility, and the thermal stability are understood as the important factors affecting reactivity. We hope to summarize the design and development of efficient oxygen carriers with high oxygen-carrying capacity and syngas selectivity, as well as contribute to the selection, design, optimization, and redox reaction mechanism of redox catalysts.

Hollow carbon sphere featuring highly dispersed Co-Nx sites for efficient and controllable syngas electrosynthesis from CO2

Electrochemical reduction of CO2 and H2O powered by green electricity provides a sustainable way to produce syngas. However, this reaction still suffers from insufficient syngas selectivity, slow charge kinetic process, and poor controllability of the CO/H2 ratio. In this work, we report a hollow carbon sphere electrocatalyst featuring highly dispersed Co-Nx sites (Co-NHCS-x) for efficient and controllable syngas electrosynthesis. The Co-NHCS-400 sample exhibits a high syngas production rate with a steady CO/H2 ratio (≈1:2) over a wide range of operating potential from −0.6 V to −1.1 V vs. RHE. The variation in synthesis temperature can finely tune the coordination environment of Co-Nx in the catalyst. Consequently, the adsorption behaviors of the CO and hydrogen atoms can be manipulated, allowing for the precise adjustment of CO and H2 proportions in the product gas. The findings are potentially applicable to the exploitation of promising carbon-based electrocatalysts for electrochemical CO2 conversion into syngas.

Enhancing CO and H2 Production in Propane Dry Reforming in Excess of CO2.

This study focuses on addressing the challenges in the dry reforming of propane, a process historically marked by low syngas yields and only moderate conversions of CO2 and propane. The primary objective was to enhance CO2 utilization and boost the selectivity of syngas (CO and H2) production using titania-based catalysts. For synthesizing these catalysts, an impregnation method was employed with subsequent characterization through X-ray diffraction (XRD), N2 adsorption-desorption, ammonia temperature-programmed desorption (TPD), and hydrogen temperature-programmed reduction (TPR). The titania-based catalysts generally possess weak acidic strength, with each catalyst displaying a unique reduction profile. The dry reforming process using these catalysts resulted in varying levels of propane conversion, with V/Ti, Ir/Ti, Al/Ti, and Zr/Ti catalysts showing distinct efficiencies. Notably, the Ir/Ti and V/Ti oxide catalysts achieved the lowest selectivity for generating intermediate byproducts such as methane, ethane, ethylene, and propylene while successfully promoting higher syngas CO and H2 production alongside stable propane conversion. When exposed to excess CO2, each catalyst consumed differing amounts of CO2 molecules. Particularly, the Ir/Ti and V/Ti oxide catalysts demonstrated enhanced activity in promoting CO2 reactions with intermediate radical species, facilitating carbon-carbon (C-C) bond dissociation and leading to increased syngas production. This study offers valuable insights into the potential of titania-based catalysts in improving the efficiency and selectivity of propane dry reforming processes for blue hydrogen.

Enhanced co-production of high-quality syngas and highly-concentrated hydrogen via chemical looping steam methane reforming over Ni-substituted La0.6Ce0.4MnO3 oxygen carriers

Chemical looping steam methane reforming (CLSMR) is increasingly attracting more and more attention as a promising technology for co-production of syngas and hydrogen. However, low reactivity, poor selectivity and weak resistance to carbon deposition of oxygen carriers (OCs) probably discourage further commercial application of CLSMR. With this background, a novel strategy of incorporating Ce and Ni into LaMnO3 is advised to promote lattice oxygen migration rate and improve syngas selectivity. The redox activity and cycle stability of La0.6Ce0.4Mn1−xNixO3 for CLSMR are explored in a fixed-bed reactor coupling with various characterization methods. The characterization results show that La0.6Ce0.4Mn1−xNixO3 OCs still maintain the standard perovskite structures and well-ordered skeleton. The introduction of Ce3+ induces large amounts of oxygen vacancies on the surface of OCs and improve the syngas selectivity of methane reforming, leading to higher oxygen mobility and lower carbon deposition. Meanwhile, the experimental results also confirm that the doping of Ni into La0.6Ce0.4MnO3 can greatly improve the oxygen-donation ability and effectively provide more active sites for reaction with methane. While excessive Ni in perovskite will enhance the methane dissociation, which is the main reason of carbon deposits. The proper amount of Ni doping can well match the methane activation rate to migration rate of bulk lattice oxygen that is feasible to realize the balance between productivity and efficiency. In addition, the reduced metal elements along with great amounts of oxygen vacancies together contribute to more active sites for the following steam splitting which avails to produce high-purity H2. La0.6Ce0.4Mn0.7Ni0.3O3 oxygen carrier eventually achieve syngas yield of 2.8 mmol/g H2 and 1.4 mmol/g CO that is closed to the ideal value without obvious carbon deposition, and pure H2 yield of 3.8 mmol/g, exhibiting the best redox performance and good regenerability. Meanwhile, La0.6Ce0.4Mn0.7Ni0.3O3 can still maintain high redox activity and basic perovskite structure after 15 cyclic redox tests, illustrating a desirable stability and reliability. In summary, this study offers a valuable and effective strategy to tackle with the bottleneck of CLSMR, paving the way of doping transition metal as a pathway of modulating reaction performance and stability of OCs in chemical looping processes.

Performance evaluation of carbon-negative syngas production via chemical looping reforming of methane from biomass pyrolysis volatiles

To realize the clean and efficient directional conversion of biomass, chemical looping reforming of biomass volatile CH4 based on a decoupling strategy is expected to carry out carbon-negative production of hydrogen-rich syngas. In this paper, a multi-functional oxygen carrier (NiFe2O4@SBA-16) for encapsulating the active metal oxide component NiFe2O4 with a three-dimensional interconnecting pore molecular sieve SBA-16 was designed. The experimental results showed that the modification strategy of composite metal oxide encapsulation improved syngas selectivity and CH4 conversion based on the fixed-bed reactor. 20 %NiFe2O4@SBA-16 showed 22.1 % CH4 conversion and 92.6 % CO selectivity under 750 °C, and it maintained good cycle stability after 15 cycles. The H2/CO ratio was effectively improved by adding part of CO2 into the feed gas, and the CH4 conversion reached over 35 %. This study provides essential data for the clean preparation of hydrogen-rich syngas from biomass and the development and design of multifunctional oxygen carriers.

Evaluation of Fe-Ni Composite Oxygen Carrier in Coal Chemical Looping Gasification

Although coal chemical looping gasification (CCLG) is a promising technology for the efficient utilization of coal, limited studies concerned about the industrial application of oxygen carrier in CCLG system owing to its performance requirements including high reactivity with solid fuel, high carbon conversion, and good mechanical property. To meet the requirements of oxygen carriers in CCLG system, novel Fe-Ni composite oxygen carrier (OC) samples were successfully prepared. The performances of these OCs were evaluated in a fixed bed reactor, where they were reduced by solid fuel and then fully oxidized by air. Both fixed bed tests and thermodynamic analysis showed that the prepare OCs exhibited high reactivity with coal and syngas selectivity, making them suitable for the CCLG process. Specifically, when the loading amount of NiO was 20 wt%, the Fe-Ni composite OCs achieved the highest carbon conversion (93.03%) and synthesis gas selectivity (73.29%). Additionally, the thermogravimetric data revealed that the Curie temperature of the OCs was higher than 550°C, making them suitable for magnetic separation of the OC particles and carbon residue in the CCLG system.

Dynamic optimal control of coal tar chemical looping gasification based on process modelling and intelligent screening

Aiming to solve the problem of low utilization and poor economic efficiency of coal tar, this study proposes a new method to convert coal tar into syngas that can be used for coal-to-oil production through chemical looping gasification reactions, thus reducing the cost of coal-to-oil production. This proposal converts tar to syngas for Fischer-Tropsch reaction through chemical looping gasification cleaning process, which is realized by process simulation and artificial intelligence prediction to ensure the stable products quality under feed jump abnormal conditions. The proposed process model is first built and the optimal operating parameters are determined by sensitivity analysis after the optimization sequence is determined from correlation analysis. A dynamic model based on the optimal steady-state model is second generated to design an optimal control scheme to efficiently deal with the unusual conditions of the feed step. The data-driven deep learning model LSTM is used to intelligently screen the optimal proportional control scheme with the advantage of low time and cost consumption. Finally, the optimal control scheme is obtained by combining the prediction results of the LSTM model and the controller additions of other important parameters, and the control effect is tested by simulating the tar feed leap conditions proves that the control6 scheme is highly resistant to disturbances. The method achieves 84.1 % high carbon conversion rate of medium-low temperature tar and 88.14 % excellent selectivity of syngas. At the same time, the adjusting of feed step condition with long-term and short-term memory network promotes the development of process design with the low time and cost consumption.

Nanoscaled Oxygen Carrier-Driven Chemical Looping for Carbon Neutrality: Opportunities and Challenges.

ConspectusClimate change poses unprecedented challenges, demanding efforts toward innovative solutions. Amid these efforts, chemical looping stands out as a promising strategy, attracting attention for its CO2 capture prowess and versatile applications. The chemical looping approach involves fragmenting a single reaction, often a redox reaction, into multiple subreactions facilitated by a carrier, frequently a metal oxide. This innovative method enables diverse chemical transformations while inherently segregating products, enhancing process flexibility, and fostering autothermal properties. An intriguing facet of this novel technique lies in its capacity for CO2 utilization in processes like dry reforming and gasification of carbon-based feeds such as natural gas and biomass. Central to the success of chemical looping technology is a profound understanding of the intricacies of redox chemistry within these processes. Notably, nanoscaled oxygen carriers have proven effective, characterized by their extensive surface area and customizable structure. These carriers hold substantial promise, enabling reactions under milder conditions.This Account offers a concise overview of the mechanisms, benefits, opportunities, and challenges associated with nanoscaled carriers in chemical looping applications, with a focus on CO2 utilization. We delve into the nuances of redox chemistry, shedding light on ionic diffusion and oxygen vacancy─two key elements that are crucial in designing oxygen carriers. This discussion extends to nanospecific factors such as the particle size effect and gas diffusivity. Through the application of density functional theory simulations, insights are drawn regarding the impact of nanoparticle size on syngas production in chemical looping. Interestingly, nanosized iron oxide (Fe2O3) carriers exhibit elevated syngas selectivity and constrained CO2 formation at the nanoscale. Moreover, the reactivity enhancement of mesoporous SBA-16 supported Fe2O3 over mesoporous SBA-15 supported Fe2O3 is elucidated through Monte Carlo simulations that emphasize the superiority of the 3-dimensional interconnected porous network of SBA-16 in enhancing gas diffusion, thereby amplifying reactivity compared to the 2-dimensional SBA-15. Furthermore, we explore prevalent nanoscaled carriers, focusing on their amplified performance in CO2 utilization schemes. These encompass the integration of nanoparticles with mesoporous supports to enhance surface area, the adoption of nanoscale core-shell architectures to enhance diffusion, and the dispersion of nanoscaled active sites on microsized carriers to accelerate reactant activation. Notably, our mesoporous-supported Fe2O3 nanocarrier facilitates methane dissociation and oxidation by reducing energy barriers, thereby promoting methane conversion. The Account proceeds to outline key challenges and prospects for nanoscaled carriers in chemical looping, concluding with a glance into future research directions. We also shine a spotlight on our research group's efforts in innovating oxygen carrier materials, supplemented by discussions on indispensable elements that are essential for successful scale-up deployment.

Pyrolytic mechanisms of typical organic components of sewage sludge in the presence of CaO: Polysaccharides, proteins, and lipids

The addition of CaO could facilitate the conversion of sewage sludge (SS) from waste to high-purity syngas. The pyrolytic characteristics of SS are a comprehensive manifestation of polysaccharides, proteins, and lipids, while the influence of CaO on their pyrolytic characteristics is rarely reported. This study conducted a thorough investigation into the pyrolytic mechanism of starch, protein, and lipid in the presence of CaO by analysing their thermal behavior, gaseous products, liquid tar, and residual char. The findings from TGA, GC, GC–MS, and FT-IR analysis indicate that the addition of CaO catalytically lowers the pyrolysis temperature of starch, protein, and lipid components and promotes their conversion into small molecules, resulting in increased syngas production. Moreover, the combination of char with the carbonation and calcination cycle of CaO leads to a significant boost in syngas (H2 and CO) yield, with up to 3 and 10 times increase from starch and protein, respectively, and a higher syngas selectivity of up to 65 %. The study also identifies those polysaccharides and proteins are the primary sources of syngas. This study can provide further insight into SS pyrolysis for syngas production in the presence of CaO and the necessary parameters to predict the pyrolysis behavior of SS in industrial applications.

Highly efficient and durable syngas production over one-step synthesized synergistic oxygen carriers in biomass chemical looping gasification

Biomass chemical looping gasification (BCLG) gives a promising platform for cost-effective and low-polluting syngas production. To overcome the cumbersome process and poor dispersion of two-step synthesized synergistic oxygen carriers (OCs), NiO-LaFeO3 synergistic OCs were synthesized in one-step by sol–gel method with the found best Ni introduction amount of 0.5. The high lattice oxygen mobility and powerful oxidation capacity derived from the Ni-Fe synergistic effect made it perform better in the BCLG reaction. Due to the extraordinary stability of crystalline phase and oxygen activity, its reactivity did not suffer from any degradation during the 50 long-time redox cycles over 2750 min under the optimal working conditions of the ex-situ configuration, mutual mode and steam/biomass mass ratio of 5.0. The gas yield, carbon conversion, syngas selectivity and H2/CO ratio were constantly maintained around 1846.45 mL/g, 86.74%, 79.96% and 2.0, respectively. This study provides a feasible technical route for highly efficient and durable syngas production.

Bi-reforming of methane in a carbon deposit-free plasmatron with high operational adaptability

An atmospheric plasmatron reactor with two-stage inlets was developed for bi-reforming of methane (CO2/CH4/H2O) to produce syngas (H2 + CO) and value-added liquid products. The influence of CH4 inlet position, gas flow rate and reactant composition were investigated. The results showed that the two-stage-inlet design allows for a wide range of operational conditions in terms of the CO2/CH4/H2O ratio (2–7:0–6:0–3) and total flow rate (4.5-11 L/min). A CO2 and CH4 conversion of 24% and 12.9%, respectively, was obtained at flow rates of up to 7-8 L/min, with no observable carbon deposit formed. A closer injection of CH4 to the core plasma area was more beneficial for both reactant conversion and syngas selectivity. Interestingly, value-added oxygenated products (e.g., methanol, ethanol, acetic acid) were produced simultaneously, offering a promising power-to-liquid (PtL) route. In particular, the direct synthesis of acetic acid from CH4 and CO2 was achieved, which is infeasible in thermocatalytic processes. A small addition of H2O (14.3%) favorably enhanced the formation of acetic acid by up to 160%, likely due to the improved generation of CH3 and COOH intermediates. Overall, this work offers a promising route for syngas and oxygenated products generation in a scalable plasmatron reactor with high operational adaptability.

Double adjustment of Ni and Co in CeO2/La2Ni2-xCoxO6 double perovskite type oxygen carriers for chemical looping steam methane reforming

Chemical looping steam methane reforming (CL-SMR) is a clean and efficient technology for the co-production of syngas and hydrogen. In this work, a series of Ni and Co doped CeO2/La2Ni2-xCoxO6 double perovskite composite oxygen carriers were developed. The introduction of Co increase a large number of surface active sites, which accelerates the surface activation of CH4, while the addition of Ni provides oxygen vacancies to promote the migration of lattice oxygen in the particles. The optimal substitution ratios of cobalt and nickel are 0.6 and 1.4, respectively. The CeO2/La2Ni1.4Co0.6O6 sample exhibits excellent syngas selectivity (95%) accompanied with high methane conversion (86%) in the methane reforming stage at 850℃, and close to 100% hydrogen concentrations in the steam oxidation stage. Density functional theory calculations demonstrated that the partial oxidation of methane is a strongly exothermic process, and the double perovskite loaded with CeO2 is more conducive to the activation of CH4 and prevents the generation of carbon deposition. The Ni-Co synergistic effect formed by the appropriate doping ratio of Ni and Co can also greatly promote the partial oxidation of methane. Subsequently, the deeply reduced metals combined with oxygen vacancies provide sufficient active stable points for water vapor cracking to generate high-purity hydrogen.

Sewage sludge steam gasification over bimetallic mesoporous Al-MCM48 catalysts for efficient hydrogen generation

This study explored the potential of steam gasification of sewage sludge over different temperatures (non-catalytic) and bimetallic (Ni–Fe and Ni–Co) mesoporous Al-MCM48 (3–5% Al basis). The higher temperature (800 °C) resulted in higher gas yield (36.74 wt%) and syngas (H2 and CO) selectivity (35.30 vol% and 11.66 vol%). Moreover, catalytic approach displayed that the Al-MCM48 was effective support because the incorporation of nickel increased the efficiency of gasification reactions compared to HZSM-5 (30). It mainly comes from the presence of mesopores and higher surface area (710.05 m2/g) providing more reaction sites and higher stability (less coke formation). Furthermore, the addition of promoters such as Co and Fe allowed the formation of Ni–Fe and Ni–Co alloys, resulting in even higher gas yield and overall H2 and CO selectivity due to the promotion of related reactions such as tar cracking, Boudouard, water gas shift and reforming and so on. Ni–Co alloy catalyst (10% Ni–5% Co/Al-MCM48) resulted in the highest H2 (∼52 vol%) selectivity due to the enhanced Ni dispersion and synergy effect between Ni and Co. Moreover, the application of bi-metal alloy on Al-MCM48 showed no coke formation and significantly reduced CO2 and hydrocarbon selectivity in the product gas. Overall, this study presented a promising solution for sewage sludge disposal in terms of clean H2 generation, reduction in CO2 and higher stability of metal based catalysts at the same time.

Enhanced syngas selectivity and carbon utilization during chemical looping reforming of methane via a non-steady redox cycling strategy

A cycling strategy is presented for simultaneous improvement of conversion and syngas selectivity during chemical looping reforming. Periodic recharging is used to re-establish a favorable nonstoichiometry profile during non-steady cycling.