APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Liguang Dou,Yadi Liu,Yuan Gao,Jiangwei Li,Xiucui Hu,Shuai Zhang,Kostya (Ken) Ostrikov,Tao Shao
Plasma-catalysis is a highly promising renewable-energy-based solution for decarbonization of industrial and environmental catalysis. However, urgent insights how to develop plasma-specific catalysts and synergize with the unique plasma effects are vitally needed for CO 2 /CH 4 utilization. Herein we provide guiding principles for catalysts design enabling discriminative production of liquid oxygenates. Comprehensive tests revealed that metallic Co was critical to enhance the CH 3 COOH generation, while oxygen vacancies (O v ) contributed to the formation of CH 3 OH. The gaseous and interfacial simulations verified the strong chemisorption of CO 2 and key O-containing radicals (O, OH, COOH) on O v , thereby shifting the reaction from high-barrier surface to the gas phase via the barrierless Eley-Rideal mechanism. The specifically O v -assisted pathways for R-COOH/R-OH generation over the custom-designed Co-MgAlO-O v multiphase structures are proposed. This study confirms that the microstructure design can modulate the radical adsorption and kinetic factors of the plasma-induced interfacial catalysis leading towards the plasma-electrified energy conversion.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Shijie Zhang,Dongren Cai,Guifen Du,Weiming Zhu,Jingliu Yang,Xiaoman Wen,Xing Yan,YiKun Zhou,Sajid Ali,Kok Bing Tan,Kang Sun,Guowu Zhan
Regulating product selectivity in CO 2 thermocatalytic hydrogenation remains challenging, particularly for shifting inherent preferences toward C 1 products. Here, we demonstrate that atomic layer deposition (ALD) of ZnO on nickel vanadate precursor (NiVO) enables a dramatic shift from methane (CH 4 ) to carbon monoxide (CO). The optimized NiVO-10ZnO-R400 (10 ALD cycles) achieves 88.1 % CO selectivity at 350°C and 0.1 MPa, surging from 1.3 % over unmodified NiVO-R400. Crucially, ALD-engineered Ni-ZnO interfaces exhibit superior CO production and stability (>200 h) compared to impregnation-synthesized counterparts, attributed to sufficient Ni-ZnO contact. Multimodal characterization and theoretical calculations reveal that ZnO-to-Ni electron transfer generates an electron-rich Ni surface, weakening CO 2 /CO adsorption and lowering surface H concentration. This suppresses the CO→CH 4 step in the CO 2 hydrogenation pathway (CO 2 →CO→CH 4 ), thereby redirecting product selectivity toward CO rather than CH 4 . Our work provides a precise interface-engineering strategy to manipulate reaction pathways for CO 2 utilization.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Ke Chen,Xin Guo,Linhan Ni,Junwen Qi,Jiansheng Li
Rational design and construction of fillers and polymers are crucial for the development of high-performance mixed matrix membranes (MMMs). In this work, amino-functionalized metal-organic frameworks KAUST-7 (KAUST-7-NH 2 ) with square-shaped sheet morphology were utilized as fillers to fabricate MMMs by physical blending with the polymer of intrinsic microporosity (PIM-1). The square-shaped KAUST-7-NH 2 sheets, prepared via in situ replacement of 2-aminopyrazine into the KAUST-7 framework, exhibited superior separation performance compared to the mono-ligand KAUST-7. Benefiting from the strong CO 2 affinity, high porosity and optimal pore sizes of KAUST-7-NH 2 , the outstanding CO 2 /CH 4 separation performance of the composite membrane was observed. The integration of square-shaped KAUST-7-NH 2 sheets provides a 2.5-fold improvement in CO 2 /CH 4 selectivity together with acceptable gas permeability as compared to the original PIM-1 membrane. Furthermore, a 100-h continuous permeation test validated the stability of the fabricated MMMs. Remarkably, the resulting MMM retained 92% of their initial CO 2 permeability after 150 days (drop of only 249 Barrer), indicating that the reduction in CO 2 permeability was approximately 10-fold lower than that of the pristine PIM-1 membrane. The prepared MMMs exhibit enhanced CO 2 /CH 4 selectivity and long-term stability, making it a highly promising candidate for practical application.
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eScience
·
2023
·
IF 0
Mi Zhang,Meng Lu,Ming-Yi Yang,Jia-Peng Liao,Yu-Fei Liu,Hao-Jun Yan,Jia-Nan Chang,Tao-Yuan Yu,Shun-Li Li,Ya-Qian Lan
Electrocatalytic CO 2 reduction (ECR) to high value-added chemicals by using renewable electricity presents a promising strategy to realize “carbon neutrality”. However, the ECR system is still limited by its low current density and poor CO 2 utilization efficiency. Herein, by using the confinement effect of covalent organic frameworks (COFs) to confine the in-situ growth of metal nanoclusters (NCs), we develop a series of Cu NCs encapsulated on COF catalysts (Cu-NC@COF) for ECR. Among them, Cu-NC@CuPc-COF as a gas diffusion electrode (GDE) achieves a maximum CO 2 -to-CH 4 Faradaic efficiency of 74 ± 3% (at −1.0 V vs. Reversible Hydrogen Electrode (RHE)) with a current density of 538 ± 31 mA cm −2 (at −1.2 V vs. RHE) in a flow cell, making it one of the best among reported materials. More importantly, the current density is much higher than the relevant industrial current density (200 mA cm −2 ), indicating the potential for industrial application. This work opens up new possibilities for the design of ECR catalysts that utilize synergistic strategy.
研究领域:
材料科学
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环境科学
·
电化学
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DOI
Catalysts
·
2026
·Vol. 16
·期 4
·327
·
IF 4.5
Biao Zhang,Liantao Yang,Boyu Chen,Yuanzhe Li,Hao Wang
Defect engineering and metal–support coupling provide an effective route to tune interfacial charge dynamics for selective photocatalytic CO2reduction. Here, Ti-vacancy-rich Bi4Ti3O12(BTvO) nanosheets were prepared and decorated with Au nanoparticles (Au NPs) to build Au-BTvO junctions that favor multi-electron/proton transfer toward deep hydrogenation. The optimized 3%Au-BTvO achieved high hydrocarbon productivity under visible light (λ > 420 nm), delivering CH4and C2H6formation rates of 92.66 and 17.96 μmol g−1h−1, respectively, with stable performance over 25 h. Spectroscopic analyses reveal higher CO2uptake and more effective surface activation, increased water adsorption with a more favorable interfacial hydration environment, and time-dependent formation of key C1and C2intermediates. In situ light-irradiation XPS, PL mapping, and KPFM collectively demonstrate directional electron transfer from Bi4Ti3O12to Au and amplified surface band bending, enabling efficient charge separation and accelerated surface reduction. This work highlights defect–metal synergy as a general strategy to boost activity, selectivity, and durability in visible-light CO2-to-methane conversion.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Nan Wang,Riguo Mei,Zhongwei Chen,Tao Yang,Xidong Lin,Qingxia Liu
Electronic-interface-confinement synergy enables full CO 2 -to-CH 4 conversion. • Achieves 65.4% CH 4 FE and 100 h stability with non-Cu catalyst, a new benchmark. • Nanoconfinement steers CO 2 -to-CH 4 by stabilizing intermediates and lowering HCOOH→HCO→H 2 CO* barrier. • S-vacancies and FeCo/Mo-edge electronic synergy boost activity and selectivity. • Topological transformation constructs tunable multi-shelled confinement nanoreactors. The electrochemical CO 2 reduction reaction (CO 2 RR) still faces critical challenges in achieving rapid product conversion and precise selectivity control due to kinetic limitations and thermodynamic competition. To overcome these limitations, this study develops a hierarchical hollow multi-shell FeCo@MoS 2 catalyst that integrates electronic modulation with nanoconfinement, thereby achieving kinetic enhancement and directional steering of methane production. This enhanced performance stems from two factors: sulfur vacancy-rich monolayer MoS 2 that enhances carrier mobility, and the synergistic effect of strong Mo-edge/FeCo coupling combined with nanoscale confinement for site stabilization. The optimized FeCo@MoS 2 -p30 (with pore size ≈30 nm) delivers a high methane Faradaic efficiency of 65.4% with 80 mA cm −2 at −1.0 V vs. RHE and exceptional operational stability for over 100 h. The computational results reveal that FeCo@MoS 2 -p30 promotes efficient methane production by steering the reaction pathway through a sequence of key intermediates. The nanoconfinement effect selectively stabilizes the adsorption of HCOO*, HCOOH*, HCO*, and H 2 CO* (favoring the HCOO* pathway over COOH), thereby redirecting the selectivity toward CH 4 . This is achieved by substantially reducing the energy barrier for the rate-determining HCOOH* → HCO* hydrogenation steps. Download: Download high-res image (167KB) Download: Download full-size image
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高影响因子
IEEE SENSORS JOURNAL
·
2026
·
IF 4.5
Weiwei Qin,Xuefeng Hu,Ming Zhou,Jilei Yang,Jiaming Liu,Peipei Li,Xiaoliang Wang,Liping Tan,Yali Bi,Wenjuan Yu,Wei Zhang
The detection of hydrogen-methane (H2-CH4) in exhaled breath takes on paramount importance for small intestinal bacterial overgrowth (SIBO) diagnosis. However, the concentrations of H2 and CH4 associated with SIBO are significantly lower, reaching only 20 and 12 ppm, respectively. Furthermore, the detection of these gases can be compromised by the presence of various volatile organic compounds (VOCs) and relative humidity (RH) in exhaled breath. In this study, a low-powered system with three high-performance tin dioxide (SnO2)-based micro-electro-mechanical system (MEMS) gas sensors for H2-CH4-VOCs detection was modified by magnetron sputtering deposition and coating, which are named as Pd/SnO2-M (M means magnetron), Pd/SnO2-C (C means coating), and SnO2-D (D means multiple doping), respectively. Particularly, the Pd/SnO2-M sensor shows excellent selectivity, high sensitivity, and low detection limitation (down to 0.033 ppm) toward H2, which is attributed to the compact grains of the film and the Pd catalysis for the dissociation of H2 molecule into two active hydrogen atoms better than other gases. In addition, the Pd/SnO2-C sensor exhibits high sensitivity and low detection limitation toward H2 (down to 0.186 ppm) and CH4 (down to 1.1 ppm) since doped Pd also gives rise to adsorbed oxygen species (Oads) above the SnO2 surface besides its catalysis. Moreover, the assembled MEMS sensor array system demonstrates gas recognition capability based on linear discriminant analysis (LDA) under controlled single-gas conditions in high-humidity environments. Then, the as-modified MEMS sensor array system is a promising platform for H2-CH4 detection.
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PubMed
高影响因子
Membranes
·
2025
·Vol. 15
·期 7
·197
·
IF 3.6
Jiale Zhang,Huixin Dong,Fei Guo,Huijun Yi,Xiaobin Jiang,Gaohong He,Wu Xiao
In this work, HNTs@ZIF-67 composites were synthesized using the in situ growth method and incorporated into 6FDA-TFMB to prepare mixed-matrix membranes (MMMs). Scanning electron microscope (SEM) and transmission electron microscope (TEM) proved that the HNTs@ZIF-67 composite not only retained the hollow structure of HNTs, but also formed a continuous ZIF-67 transport layer on the surface of HNTs. The results of gas permeability experiments showed that with the increase in HNTs@ZIF-67 incorporation, the He permeability and He/CH4selectivity of MMMs showed a trend of increasing first and then decreasing. When the loading is 5 wt%, the He permeability and He/CH4selectivity of MMMs reach 116 Barrer and 305, which are 22.11% and 79.41% higher than the pure 6FDA-TFMB membrane. The results of density functional theory (DFT) and Monte Carlo (MC) calculations reveal that He diffuses more easily inside ZIF-67, HNTs and 6FDA-TFMB than CH4, and ZIF-67 shows larger adsorption energy with He than HNTs and 6FDA-TFMB, indicating that He is easily adsorbed by ZIF-67 in MMMs. Based on experimental and molecular simulation results, the mechanism of HNTs@ZIF-67 improving the He/CH4separation performance of MMMs was summarized. With the advantage of a smaller molecular kinetic diameter, He can diffuse through ZIF-67 on the tube orifice of HNTs@ZIF-67 and enter the HNTs’ hollow tube for rapid transmission. At the same time, He can also be rapidly transferred in the continuous ZIF-67 transport channel layer, which improves the He permeability and the He/CH4selectivity of MMMs.
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PubMed
高影响因子
SOIL BIOLOGY & BIOCHEMISTRY
·
2024
·
IF 9.8
Jinzhi Yao,Minghui Xie,Linpeng Yu,Ting Liu,Tim J. Clough,Nicole Wrage-Mönnig,Jiafa Luo,Chunsheng Hu,Tida Ge,Shungui Zhou,Shuping Qin
Iron (Fe) plaque is a concentrated form of microbially available Fe oxide that coats rice plant root surfaces, representing a high density of Fe oxide and which potentially mediates paddy soil CH 4 emissions. Using a combination of methods including Fe plaque induction, isotopic labeling , pure microbial strains, and Fe oxide addition experiments, we investigated the impact of Fe plaque on methane (CH 4 ) emissions from paddy soils and explored the associated mechanisms underlying the influence of Fe plaque on CH 4 emissions. A 13 C–CH 4 isotopic labeling experiment showed that Fe plaque did not significantly affect CH 4 oxidation and associated gene expression, whereas Fe plaque significantly enriched methanogenic archaea and their expression of genes associated with methanogenesis. Pure microbial strain and Fe oxide addition experiments showed that the enhancement of CH 4 production in the presence of Fe plaque was caused by the (semi) conductive minerals within the Fe plaque, specifically, hematite , which promoted the extracellular electron transfer between the methanogenic archaea and their syntrophic bacteria, resulting in enhancement of methanogenesis. Our results imply that the presence of Fe plaque will accelerate CH 4 emissions from paddy soils and suppressing Fe plaque has the potential to mitigate CH 4 emissions.
研究领域:
环境微生物学
·
土壤学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Peng Qiu,Lei Wu,Kun Cheng,Shaowen Wu,Huiying Qi,Chunyan Xiong,Baofeng Tu
Fuel flexibility is one of the significant advantages of solid oxide fuel cells (SOFCs). The utilization of methane in SOFCs can not only reduce fuel costs, but also greatly expand its application scenarios, which is of great significance to the commercial development of SOFCs. However, when methane is directly used, Ni-based cermet anode suffers from coking, which seriously affects the durability of the cell. To alleviate the coking issue, a reforming layer outside the Ni-based anode-supporter was proposed in this study, and Ba 0.9 (Zr 0.8 Y 0.2 ) 1- x Ni x O 3-δ (BZYNi x , x = 0.05, 0.1, 0.15 and 0.2) was used as reforming layer material. Among BZYNi x catalysts, BZYNi 0.2 exhibited excellent catalytic activity toward dry reforming of methane, and methane conversion was as high as 85% at 750 °C. The excellent catalytic durability and coking-resistance of BZYNi 0.2 were also confirmed. When BZYNi 0.2 reforming layer was applied, the single cell fueled with CH 4 –CO 2 fuel showed significantly improved electrochemical performance, durability and coking-resistance. The utilization of BZYNi 0.2 reforming layer provides guidance for solving the coking issue of SOFC cermet anodes when fueled with hydrocarbon.
研究领域:
能源材料
·
催化化学
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Danxia Lin,Shi Tu,Liang Yu,Yinuo Yuan,Ying Wu,Xin Zhou,Zhong Li,Qibin Xia
The separation of light hydrocarbons like methane, ethane, and propane is an important section of the chemical industry. Herein, we reported a novel porous metal–organic framework (MOF) Cu-IPA and investigated its CH4/C2H6/C3H8 separation performance, particularly for efficient capture of C2H6 and C3H8 at low concentrations. Cu-IPA featured 1D hexagonal channels and triangular channels decorated with extensive oxygen atoms. It showed high C2H6 and C3H8 capacities in the low-pressure region, where C3H8 uptake at 5 kPa was 1.62 mmol/g and C2H6 uptake reached 1.33 mmol/g at 10 kPa, suggesting the strong adsorption affinities toward C2H6 and C3H8. For an equimolar C2H6/CH4 mixture, Cu-IPA exhibited a considerable IAST selectivity of 40, exceeding most reported MOF adsorbents. Excellent CH4/C2H6/C3H8 separation performance for Cu-IPA can be attributed to its appropriate pore size and abundant accessible oxygens atoms in the triangular channel. The molecular simulation revealed that Cu-IPA tended to form stronger C–H···O interactions with C2H6 and C3H8 due to the higher polarizabilities, resulting in larger interaction differences between C2H6/CH4 and C3H8/CH4. Breakthrough tests also supported the excellent dynamic separation performance and recyclability of Cu-IPA.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 5
·2140-2155
·
IF 4.5
Zhang Yeguang,Li Yingchao,Liu Wenxin,Li Feihu,Zhan Zili
CH 4 sensors based on metal oxide semiconductors (MOS) provide high sensitivity and fast response, but the sensitivity will be lost when they are poisoned by silicone. Therefore, there is an urgent need to address the poisoning deactivation of MOS gas sensors caused by silicone. Here, the unique strategy of coating a reactive anti-poisoning material onto the surface of the sensing material is proposed to effectively improve the anti-poisoning ability without degrading the gas sensing performance. As an experimental verification, SnO 2 /α-Al 2 O 3 is designed as the anti-poisoning layer and SnO 2 loaded with precious metals (Pt and Pd) as the sensing layer. Owing to the protection of the anti-poisoning layer, the response ( R a / R g = 24.69) and the response/recovery time (1/24 s) of the sensor to CH 4 remained undiminished at 364 °C after being poisoned under an air/hexamethyldisiloxane (HMDSO) (10 ppm) environment for 40 min, which meets the requirements of the Chinese National Standard (GB 15322.2-2019). The mechanism analysis shows that HMDSO can be decomposed with the adsorbed oxygen on the surface of SnO 2 in the anti-poisoning layer, and CH 4 can diffuse into the sensing layer to be detected. The unique anti-poisoning strategies can provide a promising insight for improving the poisoning tolerance of MOS gas sensors. Graphical abstract
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危险品化学品经营许可证（带存储）