Activity Of Catalysts Research Articles

Understanding the evolution of molybdenum-nitrogen doped carbon with long-term durability for efficient oxygen reduction reaction

The performance and durability of catalyst for Oxygen Reduction Reaction (ORR) still are challenges for fuel cell applications. Mo-NC catalyst system was established and showed the activity comparable with commercial Pt/C in alkaline conditions. An activation phenomenon during longer operation was confirmed with an obvious positive shift after 30 k cycles in accelerated degradation tests, which is rarely observed in the ORR process. The X-ray absorption fine structure (XAFS) indicated a coordination structure transform in electrochemical conditions cause the activated performance. The Density Function Theory (DFT) calculation reveals the transformation of the coordination structure is thermodynamically feasible and also conducive to lower the energy barriers of the key steps in the ORR performance, explaining the origin of the activate phenomenon. These findings give potential guidance to improve both activity and stability of catalyst.

Enhancing the activity and sulfur resistance of CuFeAlOx catalyst via the structure effect for the simultaneous removal of Hg0 and NO at wide temperature

The efficient strategy for improving SO2 resistance and catalytic activity is structural modification. Herein, the CuFeAlOx catalysts with different structures, including one-dimensionally disordered mesoporous nanoparticles structure (CuFeAl-N), one-dimensionally ordered mesoporous nanoparticles structure (CuFeAl-C), three-dimensionally ordered porous honeycomb-like structure (CuFeAl-P) and three-dimensionally ordered porous flower-like structures (CuFeAl-CP), were synthesized via a template method to investigate structure effect on activity and sulfur resistance of the catalyst for simultaneously removing NO and Hg0 at wide temperature. The results showed that the various surface characteristics resulted in distinct behaviours with regards to SO2 tolerance. CuFeAl-CP and CuFeAl-C exhibits excellent SO2 resistance, but CuFeAl-N catalyst presents poor SO2 resistance. The CuFeAl-CP with the flower-like structure possesses large specific surface area, which can expose more active sites and exhibited highly dispersed active component. More importantly, it reacts with SO2 to generate reactive sulfate providing additional acid sites, which significantly promotes high-temperature catalytic performance. One-dimensionally ordered mesoporous and three-dimensionally ordered porous effectively facilitates mass transfer of reactants and ammonium sulphate decomposition, thereby inhibiting surface sulfation and ammonium sulfate species deposition. This work lays the foundation for developing highly efficient SCR catalysts that are tolerant to SO2.

Key Role of Density Functional Approximation in Predicting M–N–C Catalyst Activities for Oxygen Reduction

Key Role of Density Functional Approximation in Predicting M–N–C Catalyst Activities for Oxygen Reduction

Diverse effects of ferromagnetic-paramagnetic phase transition on the activity and selectivity of ferromagnetic catalysts

Tuning the catalyst’s activity and selectivity is usually achieved by modifying the electronic structure through strategies such as alloying, doping, strain, and ligand modification, but inevitably accompanied by geometric structure changes of catalysts. It is challenging to modify a catalyst’s electronic structure without changing its geometric structure. Recent studies found that the second-order ferromagnetic to paramagnetic (FM-PM) phase transition could promote catalytic performance without altering the geometric structures of active sites, which was also known as the magneto-catalytic effect (MCE). However, the understanding of the MCE is still incomplete. Herein, we conducted systematic density functional theory (DFT) calculations to clarify the complex reaction mechanisms for conversions of nitrogen-containing small molecules on both FM and PM Ni (111) surfaces. Our microkinetic modeling (MKM) results demonstrate that FM-PM phase transition promotes the N2O decomposition activity of FM Ni catalyst but decreases its activity for NO decomposition while showing a negligible influence on the activity of ammonia decomposition. These results indicate the promotion, inhibition, and disappearance mechanisms of MCE on the catalytic activity, which further changes the selectivity of different products. We anticipate the MCE will work as an effective strategy for fine-tuning the activity and selectivity of ferromagnetic catalysts in heterogeneous catalysis, providing an extra basis for rational catalyst design.

Copolymerization of ethylene and isoprene initiated by metallocene catalyst

In this study, we explore the dynamic nature of metallocene catalysts during ethylene/isoprene E/IP) copolymerization, with a focus on the influence of various reaction parameters. Challenges, why do olefinic catalysts show lower activity and molecular weight (Mw) at higher temperatures and low activity with higher diene content? Firstly, we investigate the observed phenomena of decreased catalyst activity and Mw at elevated temperatures using 1.25 μmole of the metallocene. Notably, a substantial increase in active sites from 30 °C to 40 °C, reaching a peak of 89 %. Surprisingly, further temperature increments lead to a noticeable decline in active sites. At 30 °C, the active site primarily engages in the insertion of IP through 3,4 connections, with no detectable cis-1,4 or trans-1,4 connections, which suggests a lack of stereoselectivity at this temperature. At 40–50°C, cis/trans-1,4 connections and active sites are approaching a higher level. This implies a reduction in chain transfer reactions, making catalytic active sites more favorable to cis/trans-1,4 connections. Secondly, we observe a remarkable impact of IP concentration in the E/IP copolymers, active centers, and activity show stability when the amount of IP was 0.116–0.48 mol/L and then started to decline when the amount of IP 0.96 mol/L, indicating a threshold beyond which deactivation occurs. Increasing IP concentration not only reduces activity and active sites but also fails to reactivate dormant polyethylene sites. The Mw and active centers of copolymers progressively decrease with elevated IP concentration, suggesting a faster chain transfer reaction with IP compared to E.

Sulfur Vacancies are the Active Sites in the Iron Sulfide Catalyst for the Hydrogenation of Naphthalene

AbstractIron sulfide catalysts could boost the hydrogenation of polycyclic aromatic hydrocarbons, and have been widely employed in direct coal liquefaction owing to their low price and good activity. In the past, the Fe deficient structure on Fe1−xS was normally considered as the active site. Herein, the promotion effect of S vacancies on the performance in the naphthalene hydrogenation reaction was revealed. Additional S vacancies on the prepared Fe1−xS catalyst were introduced by a heat‐treatment under H2. Multiple characterization techniques verified that the density of S vacancies on catalyst surface increased with the prolonged H2 treatment time, while the Fe deficient structure displayed an opposite trend. The performance in the hydrogenation of naphthalene to tetralin was used to evaluate the catalyst activity. It was found that the sequence of naphthalene conversion over catalysts was consistent with the corresponding content of S vacancies, indicating that S vacancies were more efficient active sites. DFT calculation results revealed that both molecular H2 and naphthalene exhibited a pronounced inclination towards adsorption on S vacancies as compared to intact surface of Fe1−xS. The increasing amount of S vacancies facilitated the adsorption of reactants and the weakening of naphthalene C−C bonds.

Effect of Support Structure on the Activity of Cr-Containing Catalysts in Propane Dehydrogenation Involving CO2

Effect of Support Structure on the Activity of Cr-Containing Catalysts in Propane Dehydrogenation Involving CO2

NIR-II light-activated and Cu nanocatalyst-enabled bioorthogonal reaction in living systems for efficient tumor therapy

Bioorthogonal reaction refers to chemical reactions that occur within a biological system without interfering the normal biochemical process, offering the unprecedented versatility in engineering chemical reactions within cells. However, the precise regulation of bioorthogonal reaction in living systems is mired by the complexity of the physiological environment and the toxicity of catalysts. Herein, considering the deeper tissue penetration and reduced phototoxicity compared to visible light and ultraviolet, a second near infrared (NIR-II) light-activated Cu-based bioorthogonal reaction is developed to achieve precise spatiotemporal control and effective switching for Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) mediated chemical transformations in tumor, reducing the off-target effects. The catalytic activity of Cu catalyst through valence state interconversion between Cu(II) and Cu(I) can be precisely regulated in a reversible manner under NIR-II light irradiation-induced photoelectron transfer, which controls the extent of desired drug synthesis in bioorthogonal reaction. Meanwhile, the adverse effects of Cu(I) can be substantially mitigated within normal tissues due to their oxygen-rich condition. By utilizing NIR-II light and oxygen level, the Cu bioorthogonal catalyst achieves a balance between catalytic activity and biocompatibility. The ability to achieve precise spatiotemporal control and reversible catalysis makes this NIR-II light-mediated CuAAC platform an efficient and adaptable tool for bioorthogonal chemistry in living systems.

Impact of Nickel on Iridium-Ruthenium Structure and Activity for the Oxygen Evolution Reaction under Acidic Conditions.

Proton exchange membrane water electrolysis (PEMWE) is a promising technology to produce hydrogen directly from renewable electricity sources due to its high power density and potential for dynamic operation. Widespread application of PEMWE is, however, currently limited due to high cost and low efficiency, for which high loading of expensive iridium catalyst and high OER overpotential, respectively, are important reasons. In this study, we synthesize highly dispersed IrRu nanoparticles (NPs) supported on antimony-doped tin oxide (ATO) to maximize catalyst utilization. Furthermore, we study the effect of adding various amounts of Ni to the synthesis, both in terms of catalyst structure and OER activity. Through characterization using various X-ray techniques, we determine that the presence of Ni during synthesis yields significant changes in the structure of the IrRu NPs. With no Ni present, metallic IrRu NPs were synthesized with Ir-like structure, while the presence of Ni leads to the formation of IrRu oxide particles with rutile/hollandite structure. There are also clear indications that the presence of Ni yields smaller particles, which can result in better catalyst dispersion. The effect of these differences on OER activity was also studied through rotating disc electrode measurements. The IrRu-supported catalyst synthesized with Ni exhibited OER activity of up to 360 mA mgPGM -1 at 1.5 V vs RHE. This is ∼7 times higher OER activity than the best-performing IrO x benchmark reported in the literature and more than twice the activity of IrRu-supported catalyst synthesized without Ni. Finally, density functional theory (DFT) calculations were performed to further elucidate the origin of the observed activity enhancement, showing no improvement in intrinsic OER activity for hollandite Ir and Ru compared to the rutile structures. We, therefore, hypothesize that the increased activity measured for the IrRu supported catalyst synthesized with Ni present is instead due to increased electrochemical surface area.

The comprehensive understanding of intrinsic contribution of nickel foam as a conductive substrate in water splitting

Using nickel foam as a substrate for an electrocatalyst to report overpotential in a manuscript is a popular method in electrochemical testing or water-splitting i.e., the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER). However, use of coated Nickel foam as substrate methodology is, in essence, not reasonable for studying the intrinsic chemistry difference of electrocatalysts. To assess water-splitting devices, Ni-foam is a valid substrate if nanoparticles are grown uniformly; however, when drop-casted ink methodology is used or there is inhomogeneous growth of nanoparticles, it becomes difficult to determine whether a particular electrocatalyst is intrinsically active or not. In order to gain a rational understanding of the electrochemical activity and overpotential findings of a specific catalyst, it is essential to recognize the limitations of Ni-foam in reflecting its intrinsic role in electrocatalytic activity. In this study, the same catalyst was drop-casted on three different substrates, namely glassy carbon electrode (GCE), carbon fiber paper (CFP) and nickel foam (NF). It was observed that electrochemical results, such as overpotential, Tafel slope, turnover frequency, and others, varied significantly between NF and CFP or GCE. Therefore, it is concluded that NF should not be preferred as a conductive substrate during electrochemical testing (ET). On the contrary, other neutral substrates like CFP and GCE should be employed.

Cr dopant mediates hydroxyl spillover on RuO2 for high-efficiency proton exchange membrane electrolysis

Simultaneously improving the activity and stability of catalysts for anodic oxygen evolution reaction (OER) in proton exchange membrane water electrolysis (PEMWE) remains a notable challenge. Here, we report a chromium-doped ruthenium dioxide with oxygen vacancies, termed Cr0.2Ru0.8O2-x, that drives OER with an overpotential of 170 mV at 10 mA cm−2 and operates stably over 2000 h in acidic media. Experimental and theoretical studies show that the synergy of Cr dopant and oxygen vacancy induces an unconventional dopant-mediated hydroxyl spillover mechanism. Such dynamic hydroxyl spillover from Cr dopant to Ru active site changes the rate-determining step from OOH* formation to O2 formation and thus greatly improves the OER performance. Moreover, the Cr dopant and oxygen vacancy also play a crucial role in stabilizing surface Ru and lattice oxygen in the Ru-O-Cr structural motif. When assembled into the anode of a practical PEMWE device, Cr0.2Ru0.8O2-x enables long-term durability of over 200 h at an ampere-level current density and 60 degrees centigrade.

Decoupling Charge Carrier Electroreduction and Enzymatic CO2 Conversion to Formate Using a Dual-Cell Flow Reactor System.

With an efficient atom economy, low activation energy, and valuable applications for fuel cells and hydrogen storage, formic acid (FA) is a useful fuel product to convert CO2 and reduce emissions. Although metal catalysts are typically used for this conversion, unwanted side reactions remain a concern, particularly when products are attempted to be recovered long-term. In this study, an enzymatic catalyst is used to enable the selective conversion of CO2 to FA, as a formate ion. A dual-cell flow reactor system is used to first reduce a charge mediator electrochemically (reduction cell), which then activates a catalyst to selectively convert CO2 to formate (production cell). This approach minimizes enzyme degradation by avoiding direct contact with increased voltages and improves the quantity of formate produced. The system produced 25 mM of formate and reached over 50% Coulombic efficiency. The larger volume of this dual-cell system increases the quantity of formate produced beyond that of a batch cell. Additional design configurations are employed, including a pH control pump to maintain catalyst activity and a packed bed reactor to improve contact of the charge carrier with the catalyst. Both configurations retained higher production and efficiency long-term (∼168 h). The results highlight the challenges of developing a system where many parameters play a role in optimizing performance. Nevertheless, the ability of the system to produce formate from CO2 demonstrates the potential to improve upon this configuration for a variety of electrochemical CO2 conversion applications.

Recent Progress on Covalent Organic Frameworks Supporting Metal Nanoparticles as Promising Materials for Nitrophenol Reduction

With the utilization of nitrophenols in manufacturing various materials and the expansion of industry, nitrophenols have emerged as water pollutants that pose significant risks to both humans and the environment. Therefore, it is imperative to convert nitrophenols into aminophenols, which are less toxic. This conversion process is achieved through the use of noble metal nanoparticles, such as gold, silver, copper, and palladium. The primary challenge with noble metal nanoparticles lies in their accumulation and deactivation, leading to a decrease in catalyst activity. Covalent organic frameworks (COFs) are materials characterized by a crystalline structure, good stability, and high porosity with active sites. These properties make them ideal substrates for noble metal nanoparticles, enhancing catalytic activity. This overview explores various articles that focus on the synthesis of catalysts containing noble metal nanoparticles attached to COFs as substrates to reduce nitrophenols to aminophenols.

Enhancing the activity of Ni-B catalyst via Cu doping towards hydrogen evolution from NaBH4 hydrolysis

Developing efficient, economical, and eco-friendly catalysts for hydrogen release from hydrogen storage materials such as sodium borohydride (NaBH4) is recognized as an ideal solution to meet the growing demand for clean energy. In the present study the Ni-Cux-B alloy catalysts with different Cu doping content on the corncob (CC) substrate via a facile electroless plating method for the hydrolysis of NaBH4 were synthesized. The structural and morphological characteristics of the synthesized catalysts were investigated using various analytical techniques. The results showed that an appropriate Cu content has a remarkable excitation effect on the catalytic activity of Ni-B. The Cu doping strategy effectively changes the dispersion of metal species and provides more catalytic active sites on the surface of the catalyst. Moreover, the synergistic effect between metals after Cu doping enhances electron transfer and facilitates the adsorption and activation of BH4 and H2O molecules, thereby promoting hydrogen production activity. The optimized Ni-Cu7.2-B catalyst achieved a hydrogen generation rate (HGR) of 1321.56 mL min−1 g−1 in alkaline NaBH4 solution at 303 K, with an activation energy (Ea) of 46.26 kJ mol⁻1. The Ni-Cu7.2-B catalyst exhibits satisfactory stability, retaining 90.8 % of its initial catalytic activity after five cycles.

Boosting hydrogenation properties of supported Cu-based catalysts by replacing Cu0 active sites

Balancing the Cu+/Cu0 ratio is a common strategy to improve catalytic activity of Cu-based catalysts but is still constrained by low atomic utilization and the inherent nature of charge distribution. Herein, we reported a strategy of replacing the Cu0 active sites in Cu-based catalysts by constructing bimetallic sites on ceria, which consist of spatially separated trace amounts of palladium metal and plate-shaped Cu+ clusters with one-atom layers. The catalytic activity of the prepared Cu100Pd1/CeO2-FA catalyst (using formic acid) was 4 times that of conventional Cu100Pd1/CeO2-H catalyst in selective hydrogenation of 5-hydroxymethylfurfural to 2,5-bis(hydroxymethyl)furan, even outperforming some existing noble metal catalysts. Multiple characterizations and theoretical calculations demonstrated that the Pd atom is the heterolytic activation site for H2 molecules while plate-shaped Cu+ metal clusters act as effective hydrogenation places. This directional control involving both spatial relationship and electronic structure of the active site provides a new strategy for designing hydrogenated catalysts.

Exhaust purification of stoichiometric natural gas applications – A screening study on the impact of catalyst composition, reaction conditions and transient effects

A set of model catalysts with a variation of precious metal components comprising Pt, Pd or Pt/Pd on typical support materials (CeO2, Al2O3 and ZrO2) is evaluated in a gas mixture simulating the exhaust gas of stoichiometric natural gas-fueled engines. Three-way catalytic (TWC) performance, especially CH4 conversion, is assessed in λ-sweep as well as dynamic light-Off/light-Out tests, both with oscillating feed (1 s lean /1 s rich) implemented on a fully automated reactor system. The transient response of catalysts to changing redox potential is demonstrated in tests with varying lean/rich duration and pseudo-stationary tests. Time resolved data clearly indicate that performance and stability depend on both, precious metal composition as well as support material. Beyond screening of catalyst activity, the focus was on factors affecting the formation of undesired by-products (e.g. NH3, N2O) on hydrothermally aged catalysts. Aging severity was introduced as additional dimension in the design of the experimental study.

Asymmetric oxygen vacancies of self-supporting Co3O4/CuOx on Cu foam boosts propane total oxidation

As a low-cost and environmentally friendly transition metal oxides material, the Co3O4 has good catalytic activity for volatile organic compounds (VOCs) oxidation. However, the active components of powder cobalt-based catalysts may present uneven distribution and aggregation, thus affecting the catalytic efficiency. Herein, the Co/Cu-CF monolithic catalyst with asymmetric oxygen vacancies was developed through in-situ growth of Cu(OH)2 nanoarrays on Cu foam, which exhibits excellent performance for propane oxidation (T90 at 215 ℃). It is impressive that the catalyst shows satisfactory stability in terms of long-term, cyclic and water resistance. The results indicate that the existence of nanoarrays can provide a rich load surface and better disperse the active components, which effectively facilitates the interface interaction between cobalt and copper, inducing the generation of asymmetric oxygen vacancies. And, the activity of catalyst was significantly improved owing to the double activation effect of asymmetric oxygen vacancy on molecular oxygen and lattice oxygen. Therefore, this research offers a novel approach for designing efficient nanoarray monolithic catalysts for VOCs oxidation and other environmental applications.

Halloysite functionalized with dendritic moiety containing vitamin B1 hydrochloride as a bio-based catalyst for the synthesis of 5-hydroxymthylfurfural

Using halloysite clay and vitamin B1 hydrochloride, a novel acidic halloysite-dendrimer catalytic composite has been developed for conversion of fructose to 5-hydroxymthylfurfural. To grow the dendritic moiety on halloysite, it was first functionalized and then reacted with melamine, epichlorohydrin and vitamin B1 hydrochloride respectively. Then, the resulting composite was treated with ZnCl2 to furnish Lewis acid sites. Use of vitamin B1 as the cationic moiety of ionic liquid obviated use of toxic chemicals and resulted in more environmentally friendly composite. Similarly, dendritic moiety of generation 2 was also grafted on halloysite and the activity of both catalysts for conversion of fructose to 5-hydroxymthylfurfural was investigated to disclose the role of dendrimer generation. For the best catalytic composite, the reaction variables were optimized via RSM and it was revealed that use of 0.035 g catalyst per 0.1 g fructose at 95 °C furnished HMF in 96% yield in 105 min. Turnover numbers (TONs) and frequencies (TOFs) were estimated to be 10,130 and 5788 h−1, respectively. Kinetic studies also underlined that Ea was 22.85 kJ/mol. The thermodynamic parameters of ΔH≠\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\Delta {\ ext{H}}^{ \ e }$$\\end{document}, ΔS≠\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\Delta {\ ext{S}}^{ \ e }$$\\end{document} and ΔG≠\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\Delta {\ ext{G}}^{ \ e }$$\\end{document}, were calculated to be 23 kJ/mol, − 129.2 J/mol and 72.14 kJ/mol, respectively. Notably, the catalyst exhibited good recyclability and hot filtration approved heterogeneous nature of catalysis.

Modulating Carrier Oxygen Vacancies to Enhance Strong Oxide‐Support Interaction in IrO2/Nb2O5‐x Catalysts for Promoting Acidic Oxygen Evolution Reaction

AbstractGiven the pronounced dissolution of electrocatalysts in acidic environments, the quest for effective oxygen evolution reaction (OER) electrocatalysts suitable for proton exchange membrane (PEM) water electrolyzers persists as a formidable challenge. In this investigation, catalysts are synthesized by creating oxygen vacancies within various metal oxides (Nb2O5‐x, Ta2O5‐x, ZrO2‐x, TiO2‐x) through plasma‐assisted method, thereby facilitating the immobilization of IrO2 onto these defect‐rich surfaces. The findings unveil that IrO2/Nb2O5‐x manifests reduced overpotentials during acidic OER, achieving an overpotential down to 225 mV@10 mA cm−2, coupled with outstanding durability at multicurrent densities exceeding 200 h, attributed to strong oxide‐support interaction (SOSI) between the IrO2 catalyst and Nb2O5‐x substrate. Density functional theory (DFT) computations uncover intensified binding affinities between IrO2 and Nb2O5‐x, thus modulating the central energy levels of Ir's d orbitals toward favorable OER conditions, consequently bolstering the electrocatalytic activity and stability of the composite catalyst. Furthermore, employing IrO2/Nb2O5‐x as a PEM electrolyzer anode enables consistent operation at 1000 mA cm−2 for 200 h, with an Ir content of only 0.2852 mg cm−2 and an energy consumption of 4.34 kWh Nm−3 H2. This achievement substantially lowers the cost of hydrogen production to US$ 0.96 per kilogram, underscoring its potential for practical applications.

Effect of Mg modification on the catalytic performance of zinc malachite for methanol synthesis

The complex conditions of methanol production from coke-oven gas have brought challenges to the copper-based methanol synthesis catalyst. In this work, a series of zinc-malachite samples with different Mg contents were prepared. The zinc-malachite and calcined samples were characterized by in-situ X-ray diffraction (XRD), thermogravimetry-mass spectrometry (TG-MS), N2 physical adsorption, H2 programmed temperature reduction (H2-TPR), CO2 programmed temperature desorption (CO2-TPD) and other methods. The effects of Mg addition on the structure of zinc-malachite and its catalytic performance of methanol synthesis were investigated. The results showed that the addition of Mg increased the degree of Cu substitution inside the zinc-malachite structure and promoted the formation of high temperature carbonates in the catalyst after roasting. With the increase of Mg content, the specific surface area of the calcined catalyst increased gradually, and the Cu grain size decreased simultaneously. In-situ XRD results showed that a small amount of Mg could effectively inhibit the growth of copper grain size during the heat treatment. The evaluation showed that the initial activity of the catalyst increased first and then decreased with Mg addition, and the activity of the Mg-doped catalyst remained at a relatively high level after heat treatment. The appropriate Mg addition is beneficial to the initial activity and thermal stability of Cu-based methanol synthesis catalyst.