A Facile and Scalable Approach to Ultrathin NixMg1−xO Solid Solution Nanoplates and Their Performance for Carbon Dioxide Reforming of Methane

Carbon dioxide reforming of methane (CRM) represents a promising method that can effectively convert CH4 and CO2 into valuable energy resources. Herein, ultrathin NixMg1−xO nanoplate catalysts were synthesized using a scalable and facile process involving a one-pot, co-precipitation method in the absence of surfactants. This approach resulted in the synthesis of planar NixMg1−xO catalysts that were much thinner (˂8 nm) with larger specific surface area (>120 m2/g) in comparison to NixMg1−xO catalysts prepared by conventional methods. The ultrathin NixMg1−xO nanoplate catalysts exhibited high thermal stability, catalytic activity, and durability for CRM. Especially, these novel catalysts exhibited excellent anti-coking behavior with a low carbon deposition of 2.1 wt.% after 36 h of continuous reaction compared with the conventional catalysts, under the reaction conditions of the present study. The improved performance of the thin NixMg1−xO nanoplate catalysts was attributed to the high specific surface area and the interaction between metallic nickel nanocatalysts and the solid solution substrates to stabilize the Ni nanoparticles.


Introduction
The most abundant greenhouse gases of carbon dioxide (CO 2 ) and methane (CH 4 ) reputedly cause the climate change on a global scale. At present, controlled release and effective utilization of these reputed greenhouse gases have received considerable attention [1,2]. Carbon dioxide reforming of methane (CRM) is regarded as the most efficient processes, which can simultaneously convert CO 2 and CH 4 into hydrogen (H 2 ) and carbon monoxide (CO) (known as syngas). As we know, syngas can be widely used for chemical synthesis in many industrial applications as fuel or an intermediate. An optimal ratio of~1:1 H 2 :CO in the CRM reaction is most optimal for downstream synthesis to convert syngas into useful chemicals by subsequent reactions, such as Fisher-Tropsch reactions and oxosynthesis [3][4][5][6][7][8][9][10][11]. Unfortunately, no mature industrial technology is established for CRM, despite the potentially attractive economic and environmental incentives. That can be attributed to the lack of sustainable catalysts for CRM, most of which are quickly deactivated by the high temperature stream of CO 2 and CH 4 [2,3,12].
Although noble metals (Pt, Rh, Ir, et al.) are highly active and remarkably stable for CRM, utilization of these is limited due to their high cost and rarity [13][14][15][16][17]. By contrast, the transition metal

Catalyst Characterization
For comparing with conventional catalysts, the Ni 0.1 Mg 0.9 O-con catalysts were also prepared by Chen et al. [29] by co-precipitation method from an aqueous solution of Ni (NO 3 ) 2 ·6H 2 O and Mg (NO 3 ) 2 ·6H 2 O using K 2 CO 3 as the precipitant. In Figure 1, the XRD patterns of the Ni x Mg 1−x O catalysts containing various Ni/Mg ratios are displayed. The XRD peaks located at 2θ = 37.0 • , 42.9 • , 62.4 • , 74.8 • , and 78.6 • for all Ni x Mg 1−x O catalysts were consistent with previous reports [25,26]. It is clear from Figure 1 that the peaks indicated that the NiO-MgO solid solution was successfully prepared in the synthesis process [25,26]. Meanwhile, the XRD signal of the Ni 0.1 Mg 0.9 O-con catalysts was stronger and narrower, and, comparing with the Ni 0.1 Mg 0.9 O catalysts, indicated that the Ni 0.1 Mg 0.9 O-con catalysts have bigger crystallite size [25]. The microstructures of three synthesized catalysts were further examined using transmission electron microscopy. As shown in Figure 2a, the Ni 0.03 Mg 0.97 O catalysts displayed a thin plate-like morphology with an irregular shape and a broad particle size distribution ranging from tens to hundreds of nanometers. This feature of thin (~8 nm) could be seen in the vertically aligned nanoplates shown in Figure 2a. Increasing the concentration of Ni in the synthesis process did not lead to significant changes in morphology of the Ni 0.1 Mg 0.9 O (Figure 2b) and Ni 0.2 Mg 0.8 O (Figure 2c). Figure 2d showed that the Ni 0.1 Mg 0.9 O-con catalysts were also comprised of nanoparticles and platelet shaped. The thickness of Ni 0.1 Mg 0.9 O-con catalysts, though, was ca. 50 nm, which was obviously thicker than our catalysts.   (Table 1), respectively, which was significantly greater than that of the samples synthesized using co-precipitation methods (3~60 m 2 /g) [25,35,37]. For the Ni 0.1 Mg 0.9 O-con catalysts, the values of surface area was only 12.5 m 2 /g. Meanwhile, Figure 3a,b show the N 2 adsorption/desorption profiles and pore size distributions of the Ni x Mg 1−x O catalysts, respectively. The N 2 adsorption/desorption isotherms were type III isotherm by the IUPAC (International Union of Pure and Applied Chemistry) classification, typical of mesoporous materials. In Figure 3b, the mesopores and macropores between 2 and 100 nm of the Ni x Mg 1−x O catalysts can be observed from the pore size distributions of the catalysts.

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The strong metal-support interaction can prevent the sintering of small nickel species into big It should be mentioned that the synthesis of the binary Ni x Mg 1−x O solid solution catalysts was performed in the absence of surfactants. This can potentially avoid possible contamination induced by the surfactants or organic capping agents with subsequent high temperature annealing. To demonstrate that the synthetic method was scalable, the reaction was amplified 20 times in a 2-L Pyrex bottle. Figure 4 shows the optical graphs of a 2-L reaction and the fabricated Ni 0.1 Mg 0.9 O plates. As a result, the same properties of Ni 0.1 Mg 0.9 O plates were obtained and the yield of catalysts was about 99%. These results confirmed that the reported synthetic approach provided a facile and scalable method for the one-pot synthesis of Ni x Mg 1−x O solid solution catalysts with high surface area. H 2 -TPR (H 2 temperature-programmed reduction) properties of the Ni x Mg 1−x O solid solution catalysts ( Figure 5) were used to evaluate the reducibility of the catalysts, which contained additional information of the interaction between metallic nickel nanocatalysts and the solid solution substrates. The strong metal-support interaction can prevent the sintering of small nickel species into big particles and the coke formation. The Ni 0.03 Mg 0.97 O, Ni 0.1 Mg 0.9 O, and Ni 0.2 Mg 0.8 O catalysts showed a broad reduction peak in the range of 625-1000 • C, which was attributed to the reduction of Ni 2+ species in the crystal lattice and the formation of the metallic Ni 0 nanoparticles [37]. No reduction peaks for the catalysts could be observed at low temperatures, which precludes the existence of a free NiO phase in the catalysts, consistent with the XRD results. The Ni 0.1 Mg 0.9 O-con had two reductions, at 520 • C and 1000 • C. The first reduction peak was related to small Ni particles or to the reduction of Ni species in low interaction with MgO. The second peak was associated to strong interaction with MgO. Compared to Ni 0.1 Mg 0.9 O-con and previous literature reports, the reduction peaks of the Ni x Mg 1−x O catalysts in the range of 625-1000 • C significantly shifted toward high temperatures, demonstrating a very strong interaction between Ni and solid solution in the nanoplate catalysts [34,37]. This result indicated that Ni successfully incorporated into the structure of NiO-MgO solid solutions. at 520 °C and 1000 °C . The first reduction peak was related to small Ni particles or to the reduction 135 of Ni species in low interaction with MgO. The second peak was associated to strong interaction with demonstrating a very strong interaction between Ni and solid solution in the nanoplate catalysts 139 [34,37]. This result indicated that Ni successfully incorporated into the structure of NiO-MgO solid

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The methane conversion as a function of temperature on all catalysts is exhibited in Figure 6a. CH4   Figure 6a. CH 4 conversion was mainly dependent on the temperature of reaction. Specifically, as the reaction temperature increased, the ratio of the conversion of CH 4 increased correspondingly. As shown in Figure 6a, the methane conversion for the Ni 0.03 Mg 0.97 O catalysts was 16.4%, 33.8%, 52.6%, 68.3%, 80.3%, and 88.5%, when the reaction temperatures were 550 • C, 600 • C, 650 • C, 700 • C, 750 • C, and 800 • C, respectively, revealing the highly endothermic nature of the CRM reaction. As shown in Figure 6b, the conversion of carbon dioxide exhibited the similar tendency. The catalytic activity of the nanoplate catalysts followed the trend of Ni 0.2 Mg 0.8 O > Ni 0.1 Mg 0.9 O > Ni 0.03 Mg 0.97 O. Among these catalysts, the Ni 0.2 Mg 0.8 O catalysts exhibited the best catalytic activity, which was attributed to the higher surface area, the pore volume, and the pore size of the catalysts. For the Ni 0.1 Mg 0.9 O and Ni 0.1 Mg 0.9 O-con, the CH 4 and CO 2 conversions are shown in Figure 6a,b, exhibiting similar catalytic activity. Although the Ni 0.1 Mg 0.9 O-con had a low surface area, the similar catalytic activity with the Ni 0.1 Mg 0.9 O catalysts was shown. It was due to the additional content of Ni on the Ni 0.1 Mg 0.9 O-con catalysts' surface in low temperature (≤800 • C), which was revealed from the H 2 -TPR properties of the Ni 0.1 Mg 0.9 O and Ni 0.1 Mg 0.9 O-con catalysts.
Catalysts 2016, 6, x FOR PEER REVIEW 6 of 4 800 °C, respectively, revealing the highly endothermic nature of the CRM reaction. As shown in Figure 6b, the conversion of carbon dioxide exhibited the similar tendency. The catalytic activity of the nanoplate catalysts followed the trend of Ni0.2Mg0.8O > Ni0.1Mg0.9O > Ni0.03Mg0.97O. Among these catalysts, the Ni0.2Mg0.8O catalysts exhibited the best catalytic activity, which was attributed to the higher surface area, the pore volume, and the pore size of the catalysts. For the Ni0.1Mg0.9O and Ni0.1Mg0.9O-con, the CH4 and CO2 conversions are shown in Figure 6a,b, exhibiting similar catalytic activity. Although the Ni0.1Mg0.9O-con had a low surface area, the similar catalytic activity with the Ni0.1Mg0.9O catalysts was shown. It was due to the additional content of Ni on the Ni0.1Mg0.9O-con catalysts' surface in low temperature (≤800 °C), which was revealed from the H2-TPR properties of the Ni0.1Mg0.9O and Ni0.1Mg0.9O-con catalysts. Despite feeding equimolar amounts of CH4 and CO2 into the CRM, CO2 conversion was slightly larger than CH4 conversion at all temperatures for all catalysts. The reason for this phenomenon was the simultaneous reaction of the reverse water-gas shift reaction (RWGS) (CO2 + H2 → CO + H2O, ΔH298 = +41 KJ/mol), which led to additional amounts of CO2 and H2 being consumed to yield CO and H2O [7,16]. Figure 6c shows the plots of H2/CO ratios as a function of reaction temperature. The H2/CO ratios increased with the increase of the reaction temperature for the three catalysts. Theoretically, the ratios of H2/CO should be around 1.0. However, these ratios were less than 1 when temperature was low, which was attributed to consumption of H2 through some side reaction, such as methanation and RWGS reactions [16]. The rise of the reaction temperatures led to the increased ratio of H2/CO by Despite feeding equimolar amounts of CH 4 and CO 2 into the CRM, CO 2 conversion was slightly larger than CH 4 conversion at all temperatures for all catalysts. The reason for this phenomenon was the simultaneous reaction of the reverse water-gas shift reaction (RWGS) (CO 2 + H 2 → CO + H 2 O, ∆H 298 = +41 KJ/mol), which led to additional amounts of CO 2 and H 2 being consumed to yield CO and H 2 O [7,16]. Figure 6c shows the plots of H 2 /CO ratios as a function of reaction temperature. The H 2 /CO ratios increased with the increase of the reaction temperature for the three catalysts. Theoretically, the ratios of H 2 /CO should be around 1.0. However, these ratios were less than 1 when temperature was low, which was attributed to consumption of H 2 through some side reaction, such as methanation and RWGS reactions [16]. The rise of the reaction temperatures led to the increased ratio of H 2 /CO by facilitating the carbon gasification, water-gas shift reaction (WGS), and methane decomposition to produce more H 2 [16]. In the low temperature range (<700 • C), the H 2 /CO ratios of Ni 0.03 Mg 0.97 O were lower than those of Ni 0.1 Mg 0.9 O and Ni 0.2 Mg 0.8 O at each temperature point, indicating that small Ni nanoparticles may favor the RWGS and methanation reactions [16]. Elevating the reaction temperature resulted in a greatly increased H 2 /CO ratio on the Ni 0.03 Mg 0.97 O, reaching 0.96 and 1.06 at 750 • C and 800 • C, respectively.  Table 1) [33][34][35]38]. Therefore, they can provide enough surface areas and preserve enough active sites in the CRM reaction. The results also indicated the solid solution nanoplates with a low content of Ni and highly dispersed Ni nanocatalysts could deliver a better thermal stability in their microstructures at the high temperatures.

Durability Tests of Ni x Mg 1-x O Catalysts
In the CRM reaction, the nickel catalysts deactivated quickly due to the thermal sintering of the metallic nickel catalysts at high temperature [16,18,24]. Herein, the unexpected catalytic stability of the Ni x Mg 1−x O catalysts for the CRM reaction can be ascribed to their unique structural features and intrinsic physicochemical properties. First of all, both NiO and MgO have the face-centered cubic structure with the close lattice parameters and bond lengths [3]. Therefore, MgO and NiO can form a solid solution with a very strong interaction. This has been demonstrated by the XRD spectra ( Figure 1) and H 2 -TPR profiles ( Figure 5), which displayed a single phase of the solid solution. Due to the very strong interaction between active sites and supports, the small Ni nanocatalysts can be effectively immobilized on the surface of the solid solution and largely avoid the nickel sintering during the CRM reaction [3]. The highly stable catalytic activity of the Ni x Mg 1−x O catalysts can be maintained even after 36 hours of continuous reactions at 700 • C. To monitor the size change of the Ni 0 active component of the catalysts, the XRD patterns of the spent catalysts after 36 h continuous reactions were also recorded. In Figure 7b, the Ni 0.03 Mg 0.97 O and Ni 0.1 Mg 0.9 O catalysts revealed that the peaks of the metallic nickel phase were still weak and broad, indicating that a small amount of Ni 0 particles appeared after the continuous 36-hour reaction at the high temperature of 700 • C [40]. In contrast, the much stronger XRD peaks of the metallic Ni phase for the Ni 0.2 Mg 0.8 O and Ni 0.1 Mg 0.9 O-con catalysts were observed, indicating a serious aggregation of Ni 0 at the operational temperatures.
In order to quantify the aggregation of the Ni nanocatalysts, the integral area ratios of Ni(200) and NiMgO(220) (S Ni-200 /S NiMgO-220 ) in XRD patterns were calculated for both the freshly reduced and the spent catalysts (Figure 7). The metallic nickel aggregation of the Ni 0.03 Mg 0.97 O and Ni 0.1 Mg 0.9 O catalysts was indeed observed, as evidenced by the apparent XRD peaks of metallic nickel. As shown in Figure    Moreover, the catalytic stability of the NixMg1-xO catalysts came from MgO, a strong basic 236 support [3,41,42]. MgO as the substrate can avoid the strong acidity of the catalysts and subsequently 237 suppress the carbon deposition (discussed below) and the aggregation of the metallic nickel 238 nanocatalysts. In addition, MgO has a high thermal stability due to its very high melting point (2850    serious sintering of Ni 0 at the reaction temperature.

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Moreover, the catalytic stability of the NixMg1-xO catalysts came from MgO, a strong basic 236 support [3,41,42]. MgO as the substrate can avoid the strong acidity of the catalysts and subsequently 237 suppress the carbon deposition (discussed below) and the aggregation of the metallic nickel 238 nanocatalysts. In addition, MgO has a high thermal stability due to its very high melting point (2850     Moreover, the catalytic stability of the Ni x Mg 1-x O catalysts came from MgO, a strong basic support [3,41,42]. MgO as the substrate can avoid the strong acidity of the catalysts and subsequently suppress the carbon deposition (discussed below) and the aggregation of the metallic nickel nanocatalysts. In addition, MgO has a high thermal stability due to its very high melting point (2850 • C). As a result, MgO can keep a relatively large surface area at high temperatures compared to most oxides used as catalyst supports. Besides, the large surface areas of the catalysts provide a large amount of the reactive sites for the catalytic reaction. Although the surface areas of the three spent catalysts were reduced (Table 1), they were still larger than those of the Ni x Mg 1−x O catalysts synthesized by the conventional method and Ni 0.1 Mg 0.9 O-con. Hence, the thin nanoplate catalysts still preserved enough active sites for the efficient CRM reaction after a long, life-time testing for 36 hours at 700 • C.

Coking Characteristics of Ni x Mg 1−x O Catalysts
Carbon accumulation is another critical factor corresponding to the degradation of the CRM catalysts, in which the carbon layer deposited on the surface Ni active particles blocks the approach of the reactants towards the catalytic sites [21]. Generally, CH 4 decomposition reaction (CH 4 → C + 2H 2 , ∆H 298 = 75 kJ/mol) and CO disproportionation reaction (2CO → CO 2 + C, ∆H 298 = −172 kJ/mol) are two possible side reactions resulting in the coke formation [43,44]. The latter has been demonstrated to be the dominant mechanism of carbon deposition on Ni-based catalysts for the CRM reaction [21]. The carbon diffusion of carbon nanotubes, filamentous whisker carbon, and shell-like graphite are formed by a metal particle [33,[45][46][47]. The SEM analyses on the spent catalysts after 36 hours of CRM reactions are presented in Figure 9. For the Ni 0.03 Mg 0.97 O and Ni 0.1 Mg 0.9 O catalysts (Figure 9a,b), no obvious tubular and wire-like carbon nanostructures were observed, indicating a low carbon deposition. In contrast, the filamentous carbon was observed for the used Ni 0.2 Mg 0.8 O and Ni 0.1 Mg 0.9 O-con catalysts. Carbon accumulation is another critical factor corresponding to the degradation of the CRM 254 catalysts, in which the carbon layer deposited on the surface Ni active particles blocks the approach 255 of the reactants towards the catalytic sites [21]. Generally, CH4 decomposition reaction (CH4 → C + 256 2H2, ΔH298 = 75 kJ/mol) and CO disproportionation reaction (2CO → CO2 + C, ΔH298 = -172 kJ/mol) are 257 two possible side reactions resulting in the coke formation [43,44]. The latter has been demonstrated 258 to be the dominant mechanism of carbon deposition on Ni-based catalysts for the CRM reaction [21].

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In Figure 9d, the Ni0.1Mg0.9O-con catalysts also had the filamentous nature of the deposited coke and 278 8.1% carbon deposition. The Ni0.1Mg0.9O-con catalysts exhibited more carbon deposition than After the 36 h of continuous reactions, the temperature-programmed oxidation of the spent Ni x Mg 1−x O catalysts was also performed with the TG-DSC (Thermogravimetry-differential scanning calorimetry) techniques to estimate the coke deposition for each catalyst. The weight loss over the higher Ni content of catalysts (in Table 1 . This suggested that the Ni x Mg 1−x O catalysts with a low nickel content could significantly inhibit carbon deposition and largely maintain the higher dispersion of Ni species. The heavy carbon deposition is generally accompanied by the serious aggregation of catalysts and the decreased surface area, which are consistent with the BET measurements on the freshly reduced and the used catalysts. In Figure 9d, the Ni 0.1 Mg 0.9 O-con catalysts also had the filamentous nature of the deposited coke and 8.1% carbon deposition. The Ni 0.1 Mg 0.9 O-con catalysts exhibited more carbon deposition than Ni 0.1 Mg 0.9 O nanoplates. From the H 2 -TPR results, the Ni 0.1 Mg 0.9 O-con had Ni species in low interaction with MgO and same small Ni particles, which led to the easy sintering of Ni on Ni 0.1 Mg 0.9 O-con catalysts at high temperature. Moreover, compared with the reduced Ni 0.1 Mg 0.9 O-con catalysts, the spent Ni 0.1 Mg 0.9 O-con catalysts showed a shoulder at 44.4 • and a broad peak at 51.7 • for metallic nickel phase. These results indicated that the metallic Ni 0 particles of the Ni 0.1 Mg 0.9 O-con catalysts became bigger. Thus, it can be concluded that a strong metal-support interaction for thin Ni x Mg 1−x O nanoplates prevented the sintering of small nickel species into big particles and the coke-formation.
To further monitor the coke formation, the XRD spectra were recorded for all catalysts. In Figure 7b, strong diffraction peaks of the spent Ni 0. 2

Catalysts' Synthesis
All reagents in this research were analytical grade and used without further purification.

Synthesis of Ultrathin NixMg1-xO Solid Solution Nanoplates
The aqueous solutions of Ni (NO 3  The conventional Ni 0.1 Mg 0.9 O-con catalysts were also synthesized by co-precipitation using K 2 CO 3 as the precipitant.

Characterization
X-ray diffraction (XRD) of the catalysts were performed on a PW 1710 Philips Powder X-ray diffractometer (Philips Co. Ltd., Japan). Transmission electron microscopy (TEM) of the catalysts was analyzed at an accelerating voltage of 120 kV on a Hitachi HT7700 microscopy (Hitachi, Japan). Scanning electron microscopy (SEM) (Hitachi, Japan) of the catalysts was taken by a Zeiss Merlin system operated at 5 kV. Nitrogen adsorption and desorption measurements of the catalysts were conducted on an ASAP 2020 (Micromeritics Co. Ltd., America) apparatus. In order to ensure a clean, dry surface, the catalysts were degassed at 200 • C under vacuum. Using the Brunauer-Emmett-Teller (BET) method and the Barrett-Joyner-Halenda (BJH) method to calculate the specific surface area and the pore size distribution of the catalysts. H 2 temperature-programmed reduction (H 2 -TPR) of catalysts was operated in a quartz fixed-bed micro-reactor. Generally, 90 mg of catalysts were pretreated for 30 min at 300 • C with 30 mL/min of high-purity argon. After cooling to 25 • C, a 30 mL/min of 10% H 2 in Ar was imported and the temperature was controlled by programming with a ramping rate of 10 • C/min from room temperature to 1000 • C. The consumption of H 2 during the reduction was measured by gas chromatography (GC) equipped with a thermal conductivity detector (TCD).
The amount of carbon deposition of the used catalysts was evaluated by TG-DSC (thermogravimetry-differential scanning calorimetry) with a Netzsch STA449C thermoanalyzer (NETZSCH Co. Ltd., Germany). The spent catalysts were held in an alumina crucible for which an empty alumina crucible was taken as a reference. The temperature was heated from room temperature to 800 • C in air with a rate of 5 • C/min.

Catalytic Reaction
The catalytic activity of the samples was measured at the atmospheric pressure in a fixed-bed quartz reactor. Calcined catalysts (90 mg) were reduced in a 100 mL/min of 5% H 2 /Ar mixture at 800 • C and isothermally kept for 1 h at this temperature. The CRM was conducted with a gas composition of CH 4 :CO 2 :Ar with a 9:9:27 volume ratio and a total 45 mL·min −1 flow rate (GHSV, Gaseous Hourly Space Velocity, 30,000 mL·g −1 ·h −1 ). The catalytic activity was performed from 500 • C to 800 • C with a 5 • C/min ramping rate. For each temperature, the reaction efficiency of the catalysts was evaluated after 30 min steady state. Process gas analysis was performed by gas chromatography equipped with methanizer, TCD, FID (flame ionization detector) and the mole sieve 5A and TDX-01 columns (Stainless steel filled column). The stability of the catalysts was carried out for 36 h at 700 • C. The CH 4 and CO 2 conversions and H 2 /CO ratio were used to evaluate the properties of catalysts. The equations were as follows [40]: CH 4 conversion(%) = moles of CH 4 converted moles of CH 4 in feed × 100 CO 2 conversion(%) = moles of CO 2 converted moles of CO 2 converted in feed × 100 H 2 CO ratio = moles of H 2 produced moles of CO produced

Conclusions
In summary, the ultrathin Ni x Mg 1−x O solid solution nanoplates with high surface areas (>120 m 2 /g) were synthesized by a facile and scalable co-precipitation method. The ultrathin Ni x Mg 1−x O solid solution nanoplates displayed high catalytic activity and stability for the CRM reactions, which can be attributed to their unique physicochemical properties, providing high surface area and strong metal-support interaction to prevent coke formation and sintering of small nickel species into large particles. The characterization of the spent catalysts indicated that the Ni x Mg 1−x O solid solution nanoplate catalysts with a low nickel content can improve the thermal stability of the catalysts, preserve the small size of the metallic nickel, and resist carbon deposition. Therefore, the Ni x Mg 1−x O catalysts were prepared via a hydrothermal method exhibited good activity and stability for the CRM reaction for industrial applications.
Author Contributions: G.Z., Z.Z. conceived and designed the experiments; G.Z. and Y.W. performed the experiments; G.Z., Z.Z., and Y.W. analyzed the data; Q.K. and Y.L. contributed reagents/materials/analysis tools; G.Z. and Z.Z. wrote the paper. All authors have read and agreed to the published version of the manuscript.