Chemical Engineering Journal, Год журнала: 2023, Номер 480, С. 148195 - 148195
Опубликована: Дек. 20, 2023
Язык: Английский
Chemical Engineering Journal, Год журнала: 2023, Номер 480, С. 148195 - 148195
Опубликована: Дек. 20, 2023
Язык: Английский
Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 315, С. 121530 - 121530
Опубликована: Май 25, 2022
Язык: Английский
Процитировано
98Nature Communications, Год журнала: 2023, Номер 14(1)
Опубликована: Фев. 13, 2023
Metal promotion is the most widely adopted strategy for enhancing hydrogenation functionality of an oxide catalyst. Typically, metal nanoparticles or dopants are located directly on catalyst surface to create interfacial synergy with active sites oxide, but enhancement effect may be compromised by insufficient hydrogen delivery these sites. Here, we introduce a promote ZnZrOx methanol synthesis incorporating activation and functions through optimized integration Pd supported carbon nanotube (Pd/CNT). The CNT in Pd/CNT + system delivers activated broad area surface, factor 10 compared conventional Pd-promoted catalyst, which only transfers Pd-adjacent In CO2 methanol, exhibits drastically boosted activity-the highest among reported ZnZrOx-based catalysts-and excellent stability over 600 h stream test, showing potential practical implementation.
Язык: Английский
Процитировано
74Nature Communications, Год журнала: 2023, Номер 14(1)
Опубликована: Сен. 21, 2023
Abstract In-plane sulfur vacancies (Sv) in molybdenum disulfide (MoS 2 ) were newly unveiled for CO hydrogenation to methanol, whereas edge Sv found facilitate methane formation. Thus, selective exposure and activation of basal plane is crucial methanol synthesis. Here, we report a mesoporous silica-encapsulated MoS catalysts with fullerene-like structure atomic copper (Cu / @SiO ). The main approach based on physically constrained topologic conversion dioxide (MoO within silica. spherical curvature enables the generation strain inert plane. More importantly, few-layer can selectively expose in-plane reduce Sv. After promotion by copper, resultant Cu exhibits stable specific yield 6.11 mol MeOH Mo –1 h selectivity 72.5% at 260 °C, much superior its counterparts lacking decoration. reaction mechanism promoting role are investigated in-situ DRIFTS XAS. Theoretical calculations demonstrate that compressive facilitates formation hydrogenation, while tensile accelerates regeneration active sites, rationalizing critical strain.
Язык: Английский
Процитировано
61CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Год журнала: 2023, Номер 45, С. 162 - 173
Опубликована: Янв. 16, 2023
Язык: Английский
Процитировано
55Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(8)
Опубликована: Янв. 5, 2024
Abstract Converting CO 2 to olefins is an ideal route achieve carbon neutrality. However, selective hydrogenation light olefins, especially single‐component olefin, while reducing CH 4 formation remains a great challenge. Herein, we developed ZnZrO x /SSZ‐13 tandem catalyst for the highly of olefins. This shows C = −C and propylene selectivity up 89.4 % 52 %, respectively, suppressed down there no obvious deactivation. It demonstrated that isolated moderate Brønsted acid sites (BAS) SSZ‐13 promotes rapid conversion intermediate species derived from , thereby enhancing kinetic coupling reactions inhibit alkanes improve selectivity. Besides, weaker BAS promote intermediates into aromatics with 4–6 methyl groups, which conducive cycle. Accordingly, more propene can be obtained by elevating Si/Al ratio SSZ‐13. provides efficient strategy high
Язык: Английский
Процитировано
23ACS Catalysis, Год журнала: 2024, Номер 14(5), С. 3074 - 3089
Опубликована: Фев. 13, 2024
Understanding the relationship between catalyst structure and activity is crucial to advancing catalytic processes such as CO2 hydrogenation methanol. In this study, we investigated impact of various synthesis conditions on structural properties ZnO–ZrO2 solid solution (ZnZrOx) catalysts. By systematically adjusting drying method, calcination temperature, postsynthesis ball-milling time, use additives, synthesized a series ZnZrOx catalysts with varying surface area (4.5–106 m2 g–1) oxygen content [O/(Zn + Zr) = 1.60–2.04] similar Zn [Zn/(Zn ca. 0.20]. Our experimental computational studies revealed that methanol over structure-sensitive area-normalized positively correlated surface. The lattice (O2–) played role in H2 activation, which rate-determining step for formation; therefore, oxygen-rich regimes serve main active sites From fundamental point view, study highlights importance activity, has been previously overlooked. an engineering standpoint, our investigations suggest bearing surfaces combined high areas can exhibit desirable thus guiding rational strategy development oxide-based
Язык: Английский
Процитировано
19Industrial & Engineering Chemistry Research, Год журнала: 2024, Номер 63(14), С. 6210 - 6221
Опубликована: Март 28, 2024
Cu/ZnO/Al2O3 catalysts are widely used in methanol synthesis due to their low cost and high catalytic activity. The structural surface characteristics of Cu crucial the formation active sites for production. In this study, a series methods employed modulate catalyst structure efficiency hydrogenation CO2 methanol. A correlation activity with Cu0 area particle sizes has been established. derived from hydrotalcite-like precursor (CZA-LDH) exhibits maximum specific area, smallest size, dispersion elements, yielding largest production rate, which is comparable commercial catalyst. Stability testing shows that CZA-LDH can retain ∼94% initial situ Fourier transform infrared spectroscopy analysis indicates HCOO*, CH3O* intermediates, product CH3OH generated on surface, reaction follows formate pathway.
Язык: Английский
Процитировано
19ACS Catalysis, Год журнала: 2022, Номер 12(13), С. 7748 - 7759
Опубликована: Июнь 20, 2022
Recently, ZnxZr1–xO2–x catalysts have attracted attention as next-generation CO2-to-methanol hydrogenation catalysts. In this study, we examined the effect of Zn content on over and determined active-site structure through both calculations experiments. When was low, contained clusters (isolated [ZnOa] [ZnbOc] oligomers). The presence indicates formation Zn–O–Zr sites. Interestingly, our revealed that species in are easily exposed surface. This result is line with experimental results, suggesting were unevenly distributed surface deposited near addition excess to ZrO2 led Zn-containing ZnO nanoparticles. During reactions, sites derived from showed specific activity for hydrogenation. Understanding will lead future development
Язык: Английский
Процитировано
67Journal of Catalysis, Год журнала: 2022, Номер 407, С. 312 - 321
Опубликована: Фев. 10, 2022
Язык: Английский
Процитировано
63ACS Catalysis, Год журнала: 2023, Номер 13(20), С. 13679 - 13690
Опубликована: Окт. 10, 2023
A Cu-based catalyst has prospects for practical use in selective hydrogenation of CO2 to methanol. But the catalyst's structural complexity renders elucidation nature active sites a challenge. This work reports CuGaZrOx solid solutions with tunable Cu size scales and synergetic interactions between methanol synthesis. Atomically dispersed species (Cu1–O3) adjacent Zr site contribute enhanced capacity adsorption/activation, Ga are primarily responsible H2 dissociation over solution isolated species. Further experimental density functional theory (DFT) calculations reveal that synergy favors form CH3OH via formate pathway while suppressing undesired CO production. provides insight into structure mechanistic efficient design
Язык: Английский
Процитировано
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