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Article
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Selective sorting of hexane isomers by anion-functionalized metal-organic frameworks with optimal energy regulation
Balancing the separation selectivity and regeneration energy of alkane isomers is a daunting challenge. Here the authors utilize flexible host-guest interactions to maximize the gas-framework interactions while achieving potential energy storage to set new benchmarks for alkane isomer separation.
- Qingju Wang
- , Lifeng Yang
- & Huabin Xing
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Article
| Open Access
Well-defined diatomic catalysis for photosynthesis of C2H4 from CO2
Principal interest lies in diatomic catalysts (DACs) for efficient CO2 to C2H4 photoconversion yet optimizing catalytic performance and exploring reaction mechanisms are impeded by heteronuclear atom random distribution. Here, a novel up-bottom ion-cutting architecture is proposed for fabricating well-defined DACs.
- Zhongkai Xie
- , Shengjie Xu
- & Shuyan Song
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Article
| Open Access
Ammonia marine engine design for enhanced efficiency and reduced greenhouse gas emissions
Pilot-diesel-ignition ammonia combustion engines effective adoption is still limited by high unburned emissions and low thermal efficiency. Here, authors propose an in-cylinder reforming gas recirculation concept to improve engine thermal efficiency while reducing unburned NH3, NOx, N2O and GHG emissions.
- Xinyi Zhou
- , Tie Li
- & Wenming Yang
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Article
| Open Access
Regulating Au coverage for the direct oxidation of methane to methanol
The direct oxidation of methane to methanol occurs in two steps that are difficult to control. Here, the authors use the OH binding strength as a descriptor to optimize the trade-off effect between the two pathways over PdxAuy catalysts.
- Yueshan Xu
- , Daoxiong Wu
- & Quanbing Liu
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Article
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Lithium carbonate-promoted mixed rare earth oxides as a generalized strategy for oxidative coupling of methane with exceptional yields
Lithium carbonate-promoted mixed rare earth oxides can be used as redox catalysts for OCM at 700 °C and achieve a single-pass C2+ yield up to 30.6%. The high activity is assigned to the peroxide and OH radicals induced by Pr4+ in the redox catalyst.
- Kun Zhao
- , Yunfei Gao
- & Fanxing Li
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Article
| Open Access
Balancing elementary steps enables coke-free dry reforming of methane
High-temperature hydrocarbon conversions often face issues like coke buildup and catalyst deactivation. Here, the authors show a general approach: balancing key reaction steps to achieve coke-free processes, exemplified in a 1000-hour coke-free dry reforming of methane process by optimizing C-H activation and C removal steps.
- Jiaqi Yu
- , Tien Le
- & Wenyu Huang
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Article
| Open Access
Achieving health-oriented air pollution control requires integrating unequal toxicities of industrial particles
Health-oriented emissions reduction in China focusing on the iron and steel industry can reduce costs by 1.56 billion dollars while lowering the population-weighted toxic potency-adjusted exposure risk.
- Di Wu
- , Haotian Zheng
- & Jiming Hao
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Article
| Open Access
Mechanism of the noncatalytic oxidation of soot using in situ transmission electron microscopy
In this work, authors investigate mechanisms of noncatalytic soot oxidation and establish models applicable to different types of soot based on the particles oxidation behaviour using in-situ transmission electron microscopy.
- Ming Gao
- , Yongjun Jang
- & Fuchen Wang
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Article
| Open Access
Risk of the hydrogen economy for atmospheric methane
H2 has the potential to become the green, low-carbon fuel of the future. However, hydrogen emissions impact atmospheric methane (CH4). Bertagni et al. investigate the fate of atmospheric CH4 in scenarios of H2 economy.
- Matteo B. Bertagni
- , Stephen W. Pacala
- & Amilcare Porporato
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Article
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Ultramicroporous material based parallel and extended paraffin nano-trap for benchmark olefin purification
Selective paraffin capture to afford high-purity olefins directly is critical but still challenging. Herein, the authors discover a distinctive ultramicroporous material featuring closely packed and linearly-extended isophthalic acid units and thus serving as a paraffin nano-trap for the efficient production of ultra-high purity olefins from paraffins.
- Peixin Zhang
- , Lifeng Yang
- & Huabin Xing
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Article
| Open Access
Efficient separation of butane isomers via ZIF-8 slurry on laboratory- and pilot-scale
The separation of butane isomers, raw materials in petrochemical industry, is challenging. Here the authors report the separation of n-butane and isobutane using a metal-organic framework slurry; the separation can be performed at large scale in a pilot-scale separation tower.
- Mingke Yang
- , Huishan Wang
- & Guangjin Chen
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Matters Arising
| Open Access
Multiple induced seismicity mechanisms at Castor underground gas storage illustrate the need for thorough monitoring
- Víctor Vilarrasa
- , Silvia De Simone
- & Antonio Villaseñor
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Article
| Open Access
One-step removal of alkynes and propadiene from cracking gases using a multi-functional molecular separator
Separating mixtures of hydrocarbons of low molecular weight is desirable but challenging. Here, the authors report a porous material with responsive and self-adaptive properties that enables one-step removal of alkynes and propadiene from cracking gases.
- Qingju Wang
- , Jianbo Hu
- & Huabin Xing
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Article
| Open Access
Closing the methane gap in US oil and natural gas production emissions inventories
Methane emissions from oil and gas systems are underestimated in official inventories. Here the authors synthesize thousands of field measurements and develop an inventory-based model for a better understanding of why this underestimation exists and how it can be fixed.
- Jeffrey S. Rutherford
- , Evan D. Sherwin
- & Adam R. Brandt
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| Open Access
A tailored multi-functional catalyst for ultra-efficient styrene production under a cyclic redox scheme
Styrene is an important commodity chemical that is highly energy and CO2 intensive to produce. Here, authors report a redox-oxidative dehydrogenation scheme and a tailored core-shell redox catalyst to convert ethylbenzene to styrene with up to 91.4% single-pass yield and 82% energy savings.
- Xing Zhu
- , Yunfei Gao
- & Fanxing Li
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Article
| Open Access
Direct conversion of methane to formaldehyde and CO on B2O3 catalysts
Partial oxidation of methane to value-added C1 products remains challenging due to the favorable formation of fully-oxidized CO2. Here, the authors show supported B2O3 catalysts with tri-coordinated BO3 units as the active site are highly selective in oxidizing methane to HCHO and CO.
- Jinshu Tian
- , Jiangqiao Tan
- & Yong Wang
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Article
| Open Access
Exploiting two-dimensional morphology of molybdenum oxycarbide to enable efficient catalytic dry reforming of methane
The two-dimensional morphology of molybdenum oxycarbide (2D-Mo2COx) nanosheets dispersed on silica is found vital for the dry reforming of methane. Here the authors show that the specific activity of 2D-Mo2COx/SiO2 exceeds that of other Mo2C-based catalysts by ca. 3 orders of magnitude.
- Alexey Kurlov
- , Evgeniya B. Deeva
- & Christoph R. Müller
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Article
| Open Access
Site-dependent reactivity of MoS2 nanoparticles in hydrodesulfurization of thiophene
MoS2 nanoparticles catalyze the extraction of heteroatom S in hydrocarbons by adsorption onto S vacancies. Here, the authors show that S vacancy properties are highly site sensitive and that adsorption of thiophene leads to self-generation of a more open double vacancy site.
- Norberto Salazar
- , Srinivas Rangarajan
- & Jeppe V. Lauritsen
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Article
| Open Access
Single-atom Pt in intermetallics as an ultrastable and selective catalyst for propane dehydrogenation
Propylene production via propane dehydrogenation demands a highly stable catalyst that works without deactivation even at high temperatures. Here, the authors show that single-atom Pt included in thermally stable intermetallic PtGa works as an active and selective catalyst for propane dehydrogenation even at 600 °C for 96 h without deactivation.
- Yuki Nakaya
- , Jun Hirayama
- & Shinya Furukawa
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Article
| Open Access
Reactions of CO2 and ethane enable CO bond insertion for production of C3 oxygenates
Reacting CO2 and ethane to achieve value-added C3 oxygenates offers opportunities to simultaneously reduce CO2 emissions and upgrade underutilized ethane in shale gas. Here, the authors report a successful oxygenate production strategy enabled by inserting CO2-derived CO into ethane-derived ethylene using a tandem reactor.
- Zhenhua Xie
- , Yuanguo Xu
- & Jingguang G. Chen
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Article
| Open Access
Shale gas reserve evaluation by laboratory pyrolysis and gas holding capacity consistent with field data
Quantification of shale gas reserves is critical to shape the energy policies of countries. Here, the authors present a new procedure to estimate gas in place and show that important UK gas reserves are actually much lower than previously thought.
- Patrick Whitelaw
- , Clement N. Uguna
- & Andrew D. Carr
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Article
| Open Access
Syngas to light olefins conversion with high olefin/paraffin ratio using ZnCrOx/AlPO-18 bifunctional catalysts
Developing robust catalysts for direct synthesis of light olefins from syngas remains a challenge. Here, the authors report a novel bifunctional catalyst composed of ZnCr binary oxide and low-Si AlPO-18 zeolite which exhibits enhanced CO conversion and selectivity to C2-C4 olefins under mild reaction conditions.
- Junjie Su
- , Haibo Zhou
- & Mingyuan He
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Article
| Open Access
Direct functionalization of methane into ethanol over copper modified polymeric carbon nitride via photocatalysis
While methane is a simple, abundant feedstock for chemical industry, the selective and facile conversion to more-complex products is challenging. Here, authors show copper-containing polymeric carbon nitride to convert methane to ethanol using light under mild conditions.
- Yuanyi Zhou
- , Ling Zhang
- & Wenzhong Wang
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Article
| Open Access
China’s coal mine methane regulations have not curbed growing emissions
Chinese government has implemented regulations to reduce mining-related methane emission since 2010. Here the authors estimated methane emissions in China using GOSAT satellite observation and results reveal a business-as-usual increase in methane emissions since 2010 despite those ambitious targets.
- Scot M. Miller
- , Anna M. Michalak
- & Stefan Schwietzke
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Article
| Open Access
Promoted cobalt metal catalysts suitable for the production of lower olefins from natural gas
The conversion of natural gas to chemicals and fuels via the Fischer-Tropsch synthesis process, depends on the ability of catalyst materials to suppress the formation of methane and carbon dioxide. Here, the authors develop a Co1Mn3-Na2S catalyst, which has a hydrocarbon product spectrum deviating from the Anderson–Schulz–Flory distribution.
- Jingxiu Xie
- , Pasi P. Paalanen
- & Krijn P. de Jong
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Article
| Open Access
Deconvolution of octahedral Pt3Ni nanoparticle growth pathway from in situ characterizations
Understanding the growth pathway of faceted alloy nanoparticles at the atomic level is crucial to morphology control and property tuning, but remains a challenge. Here, the authors reveal the particle growth and facet formation mechanisms of octahedral Pt3Ni nanoparticles using multiple cutting-edge in situ techniques.
- Xiaochen Shen
- , Changlin Zhang
- & Zhenmeng Peng
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Article
| Open Access
Low carbon renewable natural gas production from coalbeds and implications for carbon capture and storage
Coalbeds produce natural gas, which has been observed to be enhanced by in situ microbes. Here, the authors add plant-derived carbohydrates (monosaccharides) to coal seams to be converted by indigenous microbes into natural gas, thus demonstrating a potential low carbon renewable natural gas resource.
- Zaixing Huang
- , Christine Sednek
- & Shengpin Li
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Article
| Open Access
Super-emitters in natural gas infrastructure are caused by abnormal process conditions
A large proportion of methane emissions from natural gas production sites are released by a fraction of high-emitting sources. Here, using Monte Carlo simulations, the authors reveal that super-emitters occur due to abnormal process conditions, explaining component and site-based inventory discrepancies.
- Daniel Zavala-Araiza
- , Ramón A Alvarez
- & Steven P. Hamburg
Direct conversion of methane to aromatics and hydrogen via a heterogeneous trimetallic synergistic catalyst