ChemSusChem
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2024
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IF 7.5
Tong Xu,Tao Shan,Yuting Jiang,Lian-hua Xu,Huiyan Zhang,Sheng Chu
Graphical Utilizing solar energy to upcycling plastic waste into value-added chemicals is a promising strategy for realizing sustainable development. In this study, an efficient photocatalytic conversion of polyethylene plastic into syngas (CO+H 2 mixtures) by using a ZnS/Ga 2 O 3 Z-scheme heterojunction photocatalyst is reported. The strategy provides a green approach to effectively mitigate plastic pollution under environmentally friendly conditions. The photocatalytic conversion of plastic waste into value-added products using solar energy presents a promising approach for promoting environmental sustainability. Nonetheless, the emission of CO 2 during the conventional photocatalytic degradation process remains a major hurdle that impedes its further development. In this study, we propose an efficient photocatalytic conversion of polyethylene plastic into syngas (CO+H 2 mixtures) by using a ZnS/Ga 2 O 3 Z-scheme heterojunction photocatalyst. It is found that the strong redox capability of photogenerated holes and electrons in the Z-scheme heterojunction photocatalyst can promote the oxidative depolymerization of PE plastic, concurrently enabling the efficient reduction of the intermediate product CO 2 into syngas. Furthermore, this system also demonstrates applicability in the conversion and upcycling of other polyolefin plastics including polypropylene and polyvinyl chloride. Our findings highlight the potential of polyolefin plastics photoreforming for the production of syngas under environmentally benign conditions.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Pengfei Song,Rong Liu,Zihan Shen,Yuwei Zhang,Xijun Li,Chenxi Zhang,Fei Wei,Yuan Liu,Chuan Wang,Zhichuan J. Xu
The catalytic synthesis of higher alcohols (HAS) from syngas is of great significance but remains profoundly challenging due to the difficulty in balancing C O cleavage, C C coupling and CO insertion. Herein, we integrate perovskite and spinel structures by doping Al into Ca 0.7 La 0.3 Ti 0.7 Co 0.3 O 3 , yielding catalysts with high selectivity for higher alcohols. The obtained Ca 0.7 La 0.3 Ti 0.7 Co 0.3 O 3 -Al x catalysts exhibit three synergistic active sites (Co 0 , Co δ+ , and oxygen vacancies) that promote C 2+ OH formation during the reaction process. Specifically, Co 0 active sites promote the dissociation of adsorbed CO and facilitate C C coupling, while Co δ+ active sites are closely associated with CO insertion. In addition, Al doping generates oxygen vacancies, and the Co Al interaction regulates both the electronic state of Co 0 surfaces and the relative abundance of Co δ+ active sites. Among the tested catalysts, Ca 0.7 La 0.3 Ti 0.7 Co 0.3 O 3 -Al 1.5 exhibited the best performance, achieving a total alcohol selectivity of 58.8%, C 2+ OH selectivity of 76.6 wt% and space-time yield (STY) of 4.3 mmol·g cat −1 ·h −1 . This work provides a potential strategy for designing catalysts for the synthesis of higher alcohols from syngas.
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Jibiao Wang,Jiansen Wang,Lingyun Yang,Houyu Zhu,Pornthip Tongying,Yuanxing Wang
Oxide-derived Cu nanowire arrays were developed for electrochemical CO 2 reduction. • Cu nanowire arrays are capable of producing syngas with a wide range of H 2 /CO ratios. • The tunable selectivity of catalysts was attributed to the grain boundaries in Cu. Electrochemical reduction of CO 2 to value-added fuels and chemical feedstocks, such as syngas, stands as an appealing solution for energy and environmental sustainability. Currently, it suffers from a lack of catalysts with good activity and selectivity. Herein, we have synthesized a series of oxide-derived Cu nanowire arrays (NAs) as catalysts for electrochemical CO 2 reduction. Copper oxides NAs were first synthesized by thermal oxidation and then electrochemically reduced. By adjusting the annealing temperatures, the obtained Cu NAs are capable of reducing CO 2 and H 2 O to produce syngas with a wide range of H 2 /CO ratios (from 2.5:1 to 0.7:1) at a low overpotential. First-principles calculations confirmed that the enhancement of CO 2 reduction and suppression of hydrogen evolution were attributed to grain boundaries in the Cu NAs. This research demonstrates a promising strategy for the development of Cu-based catalysts in tunable syngas production. Download: Download high-res image (187KB) Download: Download full-size image
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DOI
高影响因子
Journal of Energy Chemistry
·
2026
·
IF 15.6
Haoran Jia,Le Lin,Xiaohui Feng,Xiaoyue Wang,Rentao Mu,Qiang Fu
Competitive adsorption between H 2 and CO x ( x = 1, 2) on oxide catalysts represents a primary limitation in hydrogenation reactions, where mutual site blocking suppresses activity and selectivity. This constraint hampers syngas conversion and CO 2 hydrogenation, yet strategies to decouple adsorbates remain elusive. Here, we show that competitive adsorption can be overcome through a partial-site-occupation mechanism that prevents surface saturation and enables independent activation. For a model ZnCr 2 O 4 @ZnO x system, in situ infrared spectroscopy directly reveals the simultaneous adsorption of H 2 with CO or CO 2 , in contrast to the mutually exclusive adsorption observed on pristine ZnO. Kinetic measurements link this decoupling to suppressed inhibition effects and altered reaction orders, driving improved catalytic performance. Density functional theory combined with temperature-programmed analyses further demonstrates that homolytic H 2 dissociation becomes thermodynamically self-limiting, resulting in intrinsically unsaturated surface coverages. These findings indicate competitive adsorption from an inherent constraint to a tunable surface property and establish practical design strategies for cooperative activation in ZnO-based oxide-catalyzed hydrogenation reactions. The ZnCr 2 O 4 -confined ZnO x catalyst decouples the competitive adsorption between CO/CO 2 and H 2 , enabling the co-adsorption and co-activation of these small molecules. Download: Download high-res image (182KB) Download: Download full-size image
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高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-10
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IF 15.7
Feng Xiaohui,Jia Haoran,Li Rongtan,Lin Le,Li Mingrun,Chen Mingshu,Liu Chengxiang,Du Xiangze,Wang Xiaoyue,Ding Yunjie,Mu Rentao,Fu Qiang,Bao Xinhe
ZnCrO x oxides coupled with zeolites (OXZEO) allow direct conversion of syngas into light olefins, while active sites in the composite oxides remain elusive. Herein, we find that ZnO particles physically mixed with ZnCr 2 O 4 spinel particles can be well dispersed onto the spinel surfaces by treatment in syngas and through a reduction-evaporation-anchoring mechanism, forming monodispersed ZnO x species with uniform thickness or dimension on ZnCr 2 O 4 up to a dispersion threshold ZnO loading of 16.0 wt% (ZnCr 2 O 4 @ZnO x ). A linear correlation between CO conversion and surface ZnO loading clearly confirms that the ZnO x overlayer on ZnCr 2 O 4 acts as the active structure for the syngas conversion, which can efficiently activate both H 2 and CO. The obtained ZnCr 2 O 4 @ZnO x catalyst combined with SAPO-34 zeolite achieves excellent catalytic performance with 64% CO conversion and 75% light olefins selectivity among all hydrocarbons. Moreover, the ZnO x overlayer is effectively anchored on the ZnCr 2 O 4 spinel, which inhibits Zn loss during the reaction and demonstrates high stability over 100 hours. Thus, a significant interface confinement effect is present between the spinel surface and the ZnO x overlayer, which helps to stabilize ZnO x active structure and enhance the catalytic performance.
研究领域:
催化化学
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材料科学
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DOI
PubMed
高影响因子
ChemistrySelect
·
2025
·Vol. 10
·期 33
·e03600
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IF 2
Jiaqin Wang,Fang Li,Yasi Wang,Wei Huang
Graphical The Al-doped ZnO catalyst has a lower work function, which is conducive to promoting the dissociation of CH x O* to form CH x *; it also facilitates the generation of Zn x+ and oxygen vacancies, which further promotes the generation of C 2+ OH. The direct conversion of syngas into C 2+ OH has attracted significant attention as a potential pathway for energy conversion. However, this process typically requires the use of precious metals or the collaborative action of multi-component catalysts, making it relatively complex. In this paper, simple and economical Al-doped ZnO catalysts were employed for the synthesis of C 2+ OH. The results show that the work function, Zn x+, and the relative content of oxygen vacancies are linearly related to C 2+ OH/ROH. When the doping amount was 7 mol%, the catalyst had the highest C 2+ OH/ROH (82.6 wt%), corresponding to the lowest work function value, the highest Zn x+ content, and the relative content of oxygen vacancies. We reveal that the successful synthesis of C 2+ OH depends not only on the low work function of the Al-doped ZnO but also on the existence of the oxygen vacancies and Zn x+ sites. Specifically, the low work function induced by Al doping facilitates electron transfer in the reaction, facilitating the dissociation of CH x O* into CH x *. Meanwhile, the presence of oxygen vacancies enhances the dissociative adsorption capacity of CO and facilitates the formation of CH x * species. The Zn x+ sites serve as active centers for carbon chain growth, promoting C–C coupling through the insertion of CO or CH x O* into CH x *, thereby achieving chain elongation.
研究领域:
催化化学
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材料科学
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化学工程
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能量转换
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Linning Tang,Weizhuo Xu,Zhaopeng Sun,Weipeng Li,Guohao Xu,Xinyue He,Yulin Deng,Wei Sun,Bingjie Zhou,Wei Liu
Syngas (H2, CO) is a common industrial feedstock usually produced by coal gasification at high temperatures. Herein, we present an electro-coupled-chemical reforming method that converts renewable biomass carbohydrates into syngas by using lacunary phosphomolybdic acid (MoPA) as the catalyst under mild conditions (pH = 5, <100 °C). The lacunary MoPA derives from the typical Keggin structure but acts as an efficient carbohydrate C–C bond cleavage catalyst due to its active defect sites. It degrades biomass carbohydrates into C1 compounds, such as CO and CO2, with the highest kinetic rate being 22 times higher than the initial Keggin catalyst. The produced CO2 can be self-supplied into the cathode side with coupled CO2 electrocatalytic reduction for syngas yield over the typical AgPd catalyst, and simultaneously, the lacunary MoPA catalyst is regenerated at the anode side with a significant electric energy saving. In the continuous flow running for 3600 s, the current density reaches 50 mA cm–2 at −1.6 V, and the syngas can be obtained with a tunable H2:CO ratio from 2.96 to 1. Compared with conventional syngas production, the electrochemical route provides a full carbon conversion of carbohydrate biomass into syngas with the advantages of a low reaction temperature and near-neutral conditions.
研究领域:
能源化学
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催化
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电化学
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绿色化学
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生物质转化
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DOI
高影响因子
PROCEEDINGS OF THE COMBUSTION INSTITUTE
·
2026
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IF 4.6
Min Liu,Fanggang Zhang,Long Qin,Chung K. Law,Ran Sui
This work presents an experimental and mechanistic study on the catalytic partial oxidation (CPO) of n -butane for syngas production over a Rh/Al 2 O 3 catalyst. Experiments were conducted in a fixed-bed reactor under fuel-rich conditions (equivalence ratios φ = 1.5, 2.5 and 3.5) within a temperature range of 373–1073 K. The process initiates with total oxidation, seamlessly transitioning to partial oxidation and subsequently to steam/dry reforming regimes as temperature increases, with H 2 emerging as the first syngas product followed by CO and CH 4 . Based on the experimental observations, a reduced global reaction mechanism comprising eight irreversible, lumped steps was developed. Kinetic parameters were extracted from experimental data at φ = 1.5 and validated against independent datasets at φ = 2.5 and 3.5, with the model accurately capturing the major species trends. The Rh catalyst exhibits exceptional performance, achieving H 2 selectivity of 99.1% at φ = 3.5 and 873 K, surpassing reported values for methane and propane CPO systems. In addition, trace C 2-6 hydrocarbons were detected at φ = 3.5 and temperatures above 973 K, indicating the occurrence of hydrocarbon cracking under excessively fuel-rich and high-temperature conditions. XPS analysis further reveals a temperature-induced surface transition from oxidized Rh 3+ to metallic Rh 0 , which is associated with the high catalytic activity. These results provide mechanistic insight and useful kinetic parameters for modeling and optimizing Rh-catalyzed CPO of light hydrocarbons. Novelty and significance statement This work provides the first kinetic analysis and reaction mechanism for the catalytic partial oxidation (CPO) of n -butane over rhodium, addressing a significant gap in the literature, which has predominantly focused on methane and propane. The novelty lies in the elucidation of the unique two-stage reaction pathway for n -C 4 H 10 , beginning with total oxidation, sequentially transitioning through partial oxidation, and finally to reforming. A reduced reaction mechanism comprising eight lumped steps was developed, which successfully captured the species formation and the complex non-monotonic dependence on equivalence ratio and temperature. The significance of this research is that it delivers essential theoretical insights and a practical kinetic model for utilizing n -butane, a major component of LPG and NGL, in efficient syngas production. This directly advances the application of these fuels in solid-oxide fuel cell (SOFC) systems and distributed energy technologies, enhancing energy security and reducing emissions. Ultimately, this work provides guidance for the design and optimization of fuel-flexible catalytic reactors, contributing to the transition towards a more sustainable and diversified energy landscape.
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高影响因子
FUEL
·
2020
·
IF 5.578
Hao Qu,Sihui He,Yue Su,Yulong Zhang,Haiquan Su
Direct synthesis of ethanol from syngas (a mixture of H 2 and CO) is considered as an eco-friendly and industrially important process to produce renewable fuels and chemicals. The current non-noble metal catalyst systems suffer from either low selectivity or multiple processes with high energy consumption. Here, we report a novel molybdenum diselenide-based catalyst system for high-selective conversion of syngas into ethanol. For a series of K-promoted MoSe 2 catalysts with different K/Mo ratios (K x -MoSe 2 , x = 0.25-1.00), K 1.00 -MoSe 2 surprisingly exhibits excellent ethanol selectivity up to 58.7 C mol % in total alcohols and 31.1 C mol % in the total product, which is higher than the highest selectivity value for the non-noble metal catalysts reported in the literature. The high ethanol selectivity is attributed to the formation of K-Mo-Se active phase and the synergistic effect of the Mo IV , Mo V and Mo VI multivalent species in the active phase. This study opens up a highly selective non-noble metal catalyst system for the direct synthesis of ethanol by syngas, which is of practical significance for the catalytic conversion of hydrogen-poor syngas.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
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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产品关联
DOI
PubMed
高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2022
·Vol. 39
·期 7
·1744-1752
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IF 3.146
Li Feifei,Dong Jiale,Wang Mingyue,Lin Xingtao,Cai Weijie,Liu Xianyun
This work is mainly concerned with the synthesis of Co-Zn nanocomposites by employing MCM-41 silica as hard template (CoZnO-HT) and its catalytic behavior toward to CO 2 reforming with ethanol. The physicochemical features of the as-prepared catalysts were probed through various characterization techniques, including XRD, TEM, BET, H 2 -TPR, and XPS. Indeed, CoZnO-HT catalyst possessed a highly ordered mesostructure with similarity to MCM-41 template and a higher specific surface area (304 m 2 /g) compared to the reference CoZnO-C sample (4.75 m 2 /g) prepared by the conventional impregnation method. Consequently, CoZnO-HT exhibited good performance at low temperature, and full ethanol conversion could be achieved at 550 °C as well as the negligible formation of byproduct acetone. In addition, this catalyst depicted good stability and no obvious deactivation was observed after 40 h time on stream tests under the stoichiometric feed ratio. Indeed, superior specific surface area and efficient mass transport within the mesopores might be critical factors assigned to better activity and stability for CoZnO-HT.
研究领域:
催化化学
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材料科学
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能源化学
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产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Linyan Zhu,Zongze Lv,Xin Huang,Jingyu Ran,Jie Chen,Changlei Qin
Dry reforming of methane (DRM) is an efficient reaction path in converting two major greenhouse gases of CO 2 and CH 4 into valuable chemical products. However, the rapid deactivation of catalysts restricts its development to a large extent. Attempts to combat the problem have been made in this work through evaluating potential supports of La 0.7 Sr 0.3 AlO 3 and SBA-15, and understanding the confinement effect of support pores, in order to construct Ni-catalysts with high activity and durability. Results show that SBA-15 support possesses better resistance to carbon deposition than La 0.7 Sr 0.3 AlO 3 , leading to a much better catalytic performance in DRM. Moreover, Ni/SBA-15 catalyst with pores smaller than approximate 10 nm is found to be able to withstand very harsh DRM reaction conditions of GHSV = 72,000 mLg cat −1 h −1 and CH 4 /CO 2 = 1.5 for 10 h at 650 °C, and the stability of catalysts is determined to be in the order of Ni/SBA-15 > Ni/SBA-15-HC > Ni/SBA-15-TMB. The reason is suggested to be the mitigation of nickel particles aggregation due to confining pores.
研究领域:
化学工程
·
催化科学
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产品关联
DOI
高影响因子
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