Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Chen Huai,Xiong Yangyang,Li Jun,Abed Jehad,Wang Da,Pedrazo-Tardajos Adrián,Cao Yueping,Zhang Yiting,Wang Ying,Shakouri Mohsen,Xiao Qunfeng,Hu Yongfeng,Bals Sara,Sargent Edward H.,Su Cheng-Yong,Yang Zhenyu
Improving the dispersion of active sites simultaneous with the efficient harvest of photons is a key priority for photocatalysis. Crystalline silicon is abundant on Earth and has a suitable bandgap. However, silicon-based photocatalysts combined with metal elements has proved challenging due to silicon’s rigid crystal structure and high formation energy. Here we report a solid-state chemistry that produces crystalline silicon with well-dispersed Co atoms. Isolated Co sites in silicon are obtained through the in-situ formation of CoSi 2 intermediate nanodomains that function as seeds, leading to the production of Co-incorporating silicon nanocrystals at the CoSi 2 /Si epitaxial interface. As a result, cobalt-on-silicon single-atom catalysts achieve an external quantum efficiency of 10% for CO 2 -to-syngas conversion, with CO and H 2 yields of 4.7 mol g (Co) −1 and 4.4 mol g (Co) −1 , respectively. Moreover, the H 2 /CO ratio is tunable between 0.8 and 2. This photocatalyst also achieves a corresponding turnover number of 2 × 10 4 for visible-light-driven CO 2 reduction over 6 h, which is over ten times higher than previously reported single-atom photocatalysts.
研究领域:
材料科学
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催化化学
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能源转换
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DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Siyuan Zhao,Ke Ma,Kailong He,Xiaoxun Ma,Chengyi Dai
Due to cost and energy consumption constraints, converting benzene into ethylbenzene using low-cost syngas instead of ethylene as an alkylation reagent is significant. However, when using syngas as the reaction raw material, generating ethylated side chains on the benzene ring is challenging. Instead, toluene/xylene becomes the primary product. We used a three-bed series connection method in a reactor, achieving one-step high selectivity of syngas and benzene to produce ethylbenzene. In the first bed layer (ZnAl2O4/SAPO-34), the syngas was first converted into methanol/dimethyl ether (DME) on ZnAl2O4. Then, it was further converted into low-carbon olefins on SAPO-34, with the microporous shape-selective effect of SAPO-34, inhibiting the generation of toluene/xylene in the alkylation of benzene with methanol/DME. At the same time, we proved that the absence of microporous shape-selective effect acid sites on the outer surface of S34 can lead to the occurrence of side reactions of benzene and methanol/DME methylation. In the second bed layer, SAPO-34 could continue to convert unconverted methanol/DME in the first bed layer into low-carbon olefins. In the third layer (ZSM-5), ethylene and benzene underwent highly selective alkylation on ZSM-5 to convert it into ethylbenzene. We found a “volcanic” curve relationship between the selectivity of ethylbenzene and the Brønsted acid site density of ZSM-5. On the one hand, Brønsted acid could catalyze the formation of ethylbenzene from benzene and ethylene; On the other hand, excessive Brønsted acid could lead to the isomerization of ethylbenzene to toluene/xylene. When the Brønsted acid showed a site density of 0.7 mmol/g, the selectivity of ethylbenzene was as high as 87%, with a byproduct of xylene showing only 0.3%, which is usually difficult to separate from ethylbenzene. Finally, the three-bed catalytic system showed no deactivation after 100 h.
研究领域:
化学工程
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催化科学
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高影响因子
Catalysts
·
2025
·Vol. 15
·期 12
·1122
·
IF 4
Yuting Dai,Xuemin Cao,Fei Qian,Xia Li,Li Zhang,Peng He,Zhi Cao,Chang Song
The direct synthesis of long-chain α-olefins from syngas offers a strategically vital pathway for producing high-value chemicals from alternative carbon resources. However, achieving high selectivity toward C5+olefins remains challenging due to competing paraffin formation and difficulties in precisely regulating chain growth kinetics. To mitigate these critical challenges, a series of Rh-promoted Co-Mn catalysts supported on SiO2were synthesized using a carbon-mediated impregnation strategy for the direct conversion of syngas to long-chain α-olefins (C5+). The introduction of Rh significantly enhanced both catalytic activity and C5+olefin selectivity. The optimal 1.1 wt% Rh-loaded catalyst achieved 24.6% CO conversion and 46.0% total olefin selectivity, with 34.2% of the selectivity toward C5+olefins, while maintaining low CH4(6.2%) and CO2(<1%) selectivity. Comprehensive characterization techniques, including XRD, H2-TPR, XPS, and TEM/HAADF-STEM, revealed that the carbon-mediated method facilitated the formation of highly dispersed Co3O4nanoparticles with abundant oxygen vacancies and strengthened the Co-MnOxinterface. Rh promotion modulated the cobalt speciation (Co0/Co2+), improved reducibility, and enhanced the metal-support interaction. This promoted chain growth and olefin desorption while suppressing over-hydrogenation. This study demonstrates the efficacy of Rh promotion and carbon mediation in designing high-performance Fischer-Tropsch catalysts for selective α-olefin synthesis, offering new insights into the design of efficient metal-oxide interfacial catalysts.
研究领域:
催化化学
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化学工程
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材料科学
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能源与燃料
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无机化学
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DOI
高影响因子
Catalysts
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2017
·Vol. 7
·期 1
·21
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IF 3.082
Yang Han,Bo Wen,Mingyuan Zhu
In this study, we prepared core-shell structured Ni@SiO2catalysts using chemical precipitation and modified Stöber methods. The obtained Ni@SiO2samples exhibited excellent catalysis performances, including high CO conversion of 99.0% and CH4yield of 89.8%. Moreover, Ni@SiO2exhibited excellent catalytic stability during a 100 h lifetime test, which was superior to that of the Ni/SiO2catalyst. The prepared samples were characterized using a series of techniques, and the results indicated that the catalytic performance for syngas methanation reaction of the Ni@SiO2sample was markedly improved owing to its nanoreactor structure. The strong interaction between the Ni core and the SiO2shell effectively restrained the growth of particles, and the deposition of C species.Keywords:syngas methanation;Ni@SiO2;anti-carbon deposition;catalytic stability
研究领域:
化学工程
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催化材料
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DOI
高影响因子
CATALYSIS TODAY
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2019
·
IF 4.888
Huixian Zhong,Jiaming Wang,Kang An,Jie Yang,Zhi Ma,Hong Wang,Yuan Liu
A new catalyst for direct ethanol synthesis (DES) from syngas composed of Rh nanoparticles (NPs) highly dispersed on La-Ce-O modified LaFeO 3 which was loaded on SiO 2 support was studied in this work. Over the best catalyst 40.6 % of the reacted CO could be directly converted into ethanol with CO conversion of 14.2 % at 250 °C, 3 MPa and GHSV of 3900 mL (g cat h) −1 . The results indicated that adding cerium into LaFe 0.5 Rh 0.5 O 3 /SiO 2 resulted in La 1-x Ce x Fe 0.5 Rh 0.5 O 3 /SiO 2 , the incorporation of Ce effectively regulated the interface electronic states of Rh NPs . The well matched catalyzing process by the active sites of Rh 0 , Rh + (or Rh δ+ ) and the oxygen vacancies on the surface of LaFeO 3 , of those, Rh 0 dissociatively adsorbed CO and the latter two associatively adsorbed CO could effectively improve the activity and selectivity for DES. Moreover, the interaction of La-Ce-O and LaFeO 3 strengthened the CO adsorption on the oxygen vacancies on LaFeO 3 , which improved the capacity of assistance in activating CO associatively, thus further increasing the selectivity to ethanol. The catalyst exhibited excellent resistance to carbon deposition and sintering, attributing to the small size of Rh NPs and the carbon eliminating effect of La 2 O 3 and oxygen vacancies on the surface of LaFeO 3 .
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Dewang Zeng,Yu Qiu,Min Li,Li Ma,Dongxu Cui,Shuai Zhang,Rui Xiao
Chemical looping redox cycle of oxygen storage materials offers a versatile platform to convert methane to value-added products in a clean and efficient manner. However, the highly dynamic nature of the oxygen diffusion process restrains the selective formation of the target products over a long reaction period. In this work, we show the oxygen storage materials-comprising of iron oxides and zirconium oxide support, with the nickel catalyst controllably deposited—that significantly enhanced the syngas selectivity. Mechanistic study indicated the oxygen releasing rate can be well controlled within a long reaction period by the specific spatial structure, demonstrating a new strategy to tune the oxygen diffusion in chemical looping process. Through the observed spatial effects, this work can be also extended to develop more oxygen storage materials for the other chemical looping applications, e.g. methane reforming, methane oxidative coupling, ethane oxidative dehydrogenation, etc .
研究领域:
催化化学
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能源化学
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材料化学
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化学工程
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多相催化
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DOI
高影响因子
APPLIED ENERGY
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2017
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IF 7.182
Peng Lu,Jian Sun,Dongming Shen,Ruiqin Yang,Chuang Xing,Chengxue Lu,Noritatsu Tsubaki,Shengdao Shan
It is challenging to fabricate a multifunctional catalyst for consecutively catalyzing multiple reactions. Herein, we report a well-defined metal-zeolite interface derived from a CuZnAl@H-Beta core@shell catalyst to realize one-step syngas conversion to liquefied petroleum gas (LPG). The multifunctional interface between CuZnAl core and H-Beta zeolite shell is composed of Cu and acid zeolite with a content gradient, through which synthesized methanol via syngas on the core will pass. The interface is able to catalyze the tandem dehydration of methanol to olefins on acid sites and olefin hydrogenation to C 3–4 saturated hydrocarbons (LPG fraction) over exposed Cu sites on the interface instead of noble metals in conventional catalysts. The selectivity of LPG in hydrocarbons over the prepared capsule catalyst reaches as high as 77% accompanied by a record low methane and C 2 selectivity (<2.0%).
研究领域:
催化化学
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化学工程
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材料科学
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能源转换
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DOI
高影响因子
WASTE MANAGEMENT
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2019
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IF 5.431
Hongcai Su,Ekkachai Kanchanatip,Defeng Wang,Rendong Zheng,Zhicheng Huang,Yang Chen,Ishrat Mubeen,Mi Yan
In China, waste sorting practice is not strictly followed, plastics, especially food packaging, are commonly mixed in food waste. Supercritical water gasification (SCWG) of unsorted food waste was conducted in this study, using model unsorted food waste by mixture of pure food waste and plastic. Different operating parameters including reaction temperature, residence time, and feedstock concentration were investigated. Moreover, the effect of three representative food additives namely NaCl, NaHCO 3 and Na 2 CO 3 were tested in this work. Finally, comparative analysis about SCWG of unsorted food waste, pure food waste, and plastic was studied. It was found that higher reaction temperature, longer residence time and lower feedstock concentration were advantageous for SCWG of unsorted food waste. Within the range of operating parameters in this study, when the feedstock concentration was 5 wt%, the highest H 2 yield (7.69 mol/kg), H 2 selectivity (82.11%), total gas yield (17.05 mol/kg), and efficiencies of SCWG (cold gas efficiency, gasification efficiency, carbon gasification efficiency, and hydrogen gasification efficiency) were obtained at 480 °C for 75 min. Also, the addition of food additives with Na + promoted the SCWG of unsorted food waste. The Na 2 CO 3 showed the best catalytic performance on enhancement of H 2 and syngas production . This research demonstrated the positive effect of waste sorting on the SCWG of food waste, and provided novel results and information that help to overcome the problems in the process of food waste treatment and accelerate the industrial application of SCWG technology in the future.
研究领域:
环境科学
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能源工程
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2026
·
IF 5.1
Hanlin Wang,Xianglin Chen,Yafei Guo,Pu Huang,Antian Wang,Jingyi Shi,Huaxiang Gao,Ruilin Wang,Chuanwen Zhao
Electrochemical CO 2 reduction to syngas driven by renewable energy offers a sustainable alternative to conventional fossil-fuel-based processes, while maintaining a stable H 2 /CO ratio under the inherently fluctuating potentials remains a substantial challenge. In this study, a series of supported Zn catalysts are fabricated by electrodepositing Zn onto Cu foil substrates, with a systematic investigation into the effects of deposition current density (−5 to −20 mA/cm 2 ) and deposition time (10 to 20 min) on catalyst structure and performance. Characterization results reveal that, with increasing deposition parameters, Zn species evolve from discrete nanoplates into an interwoven network of wrinkled structures, accompanied by decreased work function and charge transfer resistance. The synthesized catalysts exhibit a favorable balance in activity toward the electrochemical CO 2 reduction reaction (eCO 2 RR) and hydrogen evolution reaction (HER), thereby enabling highly tunable syngas production with H 2 /CO ratios ranging from 0.5 to 5.4. Notably, the Cu-Zn catalysts demonstrate remarkable stability in syngas composition, maintaining a nearly constant H 2 /CO ratio across a wide potential window of −1.11 to −1.41 V vs. reversible hydrogen electrode (RHE). Furthermore, the Cu-Zn-10–10 catalyst exhibits excellent durability under fluctuating voltage conditions over 24 h, highlighting its potential for seamless integration with intermittent green electricity. In-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and density functional theory (DFT) calculations indicate that the Cu-Zn bimetallic sites moderately enhance *CO adsorption, inhibiting its rapid desorption. Moreover, the energy barriers of eCO 2 RR and HER show little variation with potential, which collectively ensure the stability of the H 2 /CO ratio within the range of −1.11 to −1.41 V vs. RHE.
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高影响因子
CHEMICAL ENGINEERING & TECHNOLOGY
·
2026
·Vol. 49
·期 4
·e70205
·
IF 2
Yu-Qing Li,Yuwei Wang,Fei Wang,Hong Chen,Shenghao Yang,Lihong Zhao,Xu Liang,Yuanli Jiang,Feidong Xie,Liutao Hou,Zhenfeng Liu,Jiantang Sun
A structured, chloride-free Pd–Cu/NaY catalyst was developed for the direct synthesis of dimethyl carbonate (DMC) from syngas-derived methyl nitrite and CO. The NaY zeolite support stabilizes Pd(II) species via strong electrostatic interactions, while Cu addition enhances durability by suppressing Pd reduction and aggregation, as confirmed by H 2 -TPR and TEM. Using shaped spherical supports improves DMC selectivity by limiting methyl nitrite decomposition side reactions through diffusion constraints. Under optimized conditions (CO/MN = 1/6, 120°C), the catalyst achieves a DMC space-time yield of 669 g·kg −1 ·h −1 with high selectivity. A 1000 h stability test shows sustained activity above 550 g·kg −1 ·h −1 after an initial run-in period. In situ DRIFTS studies identify the ligand exchange step as rate-determining and elucidate the full reaction pathway. This robust catalytic system demonstrates strong potential for pilot-scale and industrial syngas-to-DMC processes.
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2026
·
IF 6.6
Liyan Wang,Xiaojun Yang,Yuhang Tan,Yu Li,Zhipeng Wang,Jian Song
Due to the complicated component of ZnCr oxides, the function of the active phases remains controversy, limiting its improvement of catalytic performance for converting syngas to higher alcohols. Herein, a series of ZnCr catalysts with tunable ZnO/ZnCr 2 O 4 molar ratios were fabricated via ball milling of the two individual oxides. Within the ZnO:ZnCr 2 O 4 range of 1:1 to 0.5:1, both CO conversion (18.5%) and isobutanol selectivity (29.0%) were significantly enhanced, while the water‑gas shift reaction and hydrocarbon formation were effectively suppressed. This improved performance originated from synergistic interface effects as revealed by the systematic characterization (XPS, CO‑TPD, and in situ DRIFTS etc.). Lattice distortion and electronic interaction at the interface induced the producing of octahedrally coordinated Zn 2+ sites on ZnCr 2 O 4 , strengthening CO adsorption, meanwhile, ZnO promoted interface hydrogen migration and hydroxyl cycling, steering the CHO* intermediate formation and facilitating C–C coupling. Furthermore, the electron‑rich lattice oxygen at the interface, with moderate basicity, served as active sites for β addition reaction of C 2 intermediate and carbon‑chain growth. These findings clarify the critical role of dual‑phase interface structure in regulating the reaction pathway during syngas conversion, providing a new strategy for the design of high‑performance catalysts for isobutanol synthesis.
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2025
·
IF 6.9
Shiqi Li,Liang Fu,Zhenping Qu,Mengyuan Qin,Lingling Zhou
Zn-based catalysts are attractive candidates for electrocatalytic CO 2 reduction to syngas, yet their unstable structure and narrow syngas ratio limit the application. In this work, the Ga 2 O 3 /ZnO (GZO) catalyst with stable dual active sites was prepared for tunable CO/H 2 ratio (0.21 ∼ 3.07) production over a wide potential range (−0.79 ∼ −1.29 V vs. RHE). The Ga 2 O 3 decoration could tailor the electronic structure of ZnO and boost the generation of oxygen vacancies (O V ) in the catalyst, thus enhancing the adsorption of CO 2 and the transportation of electrons, further improving CO selectivity at low potentials. Meanwhile, at high potential, Ga 2 O 3 would dominate the promotion of hydrogen evolution reaction (HER). As a result, the GZO catalyst led to the tunable syngas, and the syngas ratio varied upon changing the applied potentials and Ga 2 O 3 content. This work provided new possibilities for the development of advanced catalytic systems for various syngas industrial applications.
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高影响因子
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