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| Open AccessReprogramming biocatalytic futile cycles through computational engineering of stereochemical promiscuity to create an amine racemase
Racemization of chiral amines poses a challenge, making dynamic kinetic resolution inaccessible for industrial applications. Here, the authors demonstrate in silico engineering of an amine transaminase to create a new-to-nature amine racemase.
- Sang-Woo Han
- , Youngho Jang
- & Jong-Shik Shin
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Article
| Open AccessNanowire-assisted electrochemical perforation of graphene oxide nanosheets for molecular separation
The permeation pathway length and tortuosity of nanosheet membranes are usually extremely large. Here, a facile, scalable, and controllable nanowire electrochemical concept is reported for perforating and modifying nanosheets to shorten permeation pathway and adjust transport property.
- Hai Liu
- , Xinxi Huang
- & Wanbin Li
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| Open AccessOrganohydrogel-based transparent terahertz absorber via ionic conduction loss
Transparent absorbers for electromagnetic interference shielding are sought in the terahertz frequency range. The authors demonstrate organohydrogel-elastomer composites based on permittivity gradients, with strong ionic conduction loss, showing high absorption in the 0.5–4.5 THz band.
- Wenke Xie
- , Qian Tang
- & Qiye Wen
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Article
| Open AccessRoll-to-plate 0.1-second shear-rolling process at elevated temperature for highly aligned nanopatterns
In this work, authors demonstrate a 0.1-second shear rolling process capable of shearing without peeling up to 280 °C. This enables roll-to-plate fabrication of highly and unidirectionally aligned sub−10 nm block copolymer patterns over large wafer areas.
- Junghyun Cho
- , Jinwoo Oh
- & Jeong Gon Son
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Article
| Open AccessPolyMOF nanoparticles constructed from intrinsically microporous polymer ligand towards scalable composite membranes for CO2 separation
Microporous polymer ligand provides particle size reduction, enhanced ultramicroporosity (3–4 Å), and better colloidal stability in the polymer–metal–organic framework (polyMOF) system. This leads to defect-free and scalable composite membranes for efficient CO2 separation.
- Tae Hoon Lee
- , Byung Kwan Lee
- & Ho Bum Park
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Article
| Open AccessEnhanced formation of methane hydrate from active ice with high gas uptake
Gas hydrates have promising energy storage applications, a main bottleneck being their slow formation kinetics. Here, the authors demonstrate that by dispersing kinetic promoters in porous ice as active ice for gas hydrate formation, a minute-level formation process can be achieved for hydrate-based technologies.
- Peng Xiao
- , Juan-Juan Li
- & Guang-Jin Chen
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Article
| Open AccessEnabling direct-growth route for highly efficient ethanol upgrading to long-chain alcohols in aqueous phase
Achieving efficient carbon chain propagation remains a grand challenge for ethanol upgrading. Here, the authors report sulfur doped Ni@C-Sx catalysts with controllably exposed nickel sites that can dramatically improve direct-growth probability towards long-chain alcohols production.
- Juwen Gu
- , Wanbing Gong
- & Yujie Xiong
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Article
| Open AccessDesign for improving corrosion resistance of duplex stainless steels by wrapping inclusions with niobium armour
Nonmetallic inclusions often induce serious corrosion failure of steel, causing catastrophic accidents and economic losses. Here, the authors propose a strategy of wrapping deleterious inclusions with niobium armour (Z phase), improving the corrosion resistance of duplex stainless steel.
- Shucai Zhang
- , Hao Feng
- & Guoping Li
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Article
| Open AccessProgrammable catalysis by support polarization: elucidating and breaking scaling relations
Can support polarisation introduce an extra degree of freedom in catalyst scaling relations? This research considers a computational approach for studying catalysts on polar supports and identifies the origin of broken scaling relations.
- Seongjoo Jung
- , Cristina Pizzolitto
- & Turan Birol
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Article
| Open AccessFunctional Janus structured liquids and aerogels
A combination of functional nanoparticles and liquid streaming can be used to generate structures for the fabrication of soft functional materials. In this study, authors demonstrate the creation of Janus-structured liquids with anisotropic and programmable distributions of nanoparticles by utilizing interfacial assembly and jamming of nanoparticles at the liquid-liquid interface.
- Ahmadreza Ghaffarkhah
- , Seyyed Alireza Hashemi
- & Mohammad Arjmand
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Article
| Open AccessLithium 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 AccessSteam recovery from flue gas by organosilica membranes for simultaneous harvesting of water and energy
Flue gas is a rich source of water and energy. Here, authors provide a state-of-the-art system anchored in organosilica membrane technology, attaining impressive steam recovery, delivering up to 70% energy recovery, and offering a promising remedy for global water shortages.
- Norihiro Moriyama
- , Akihiro Takeyama
- & Toshinori Tsuru
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| Open AccessOperando Li metal plating diagnostics via MHz band electromagnetics
Internal growth of Li-metal deposition is critical for evaluating the state of safety in lithium-ion batteries. Here the authors show a Li-metal detection method utilizing high-frequency electromagnetics, which can be assembled as a sensor for monitoring cycle-by-cycle growth of Li-metal plating.
- Masanori Ishigaki
- , Keisuke Ishikawa
- & Tsuyoshi Sasaki
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Article
| Open AccessElectrocatalytic valorization of lignocellulose-derived aromatics at industrial-scale current densities
The authors report a flow-cell system equipped with highly-electrolyte permeable Rh diffusion cathode for electrocatalytic hydrogenation of important bio-oil aromatic molecules at industrial-scale current densities.
- Tao Peng
- , Wenbin Zhang
- & Wei Zhao
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| Open AccessCeramic thin-film composite membranes with tunable subnanometer pores for molecular sieving
Ceramic membranes are a promising alternative to polymeric membranes for selective separations, given their ability to operate under harsh chemical conditions. Here authors demonstrate a molecular-level design of ceramic membranes with tunable subnanometer pores.
- Xuechen Zhou
- , Rahul Shevate
- & Menachem Elimelech
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Article
| Open AccessGeneralised analytical method unravels framework-dependent kinetics of adsorption-induced structural transition in flexible metal–organic frameworks
The kinetics of guest-induced structural transition shown by flexible metal–organic frameworks (MOFs) remain poorly understood despite being crucial for process design. Here, three MOFs are studied to reveal the framework-dependent kinetic nature.
- Yuta Sakanaka
- , Shotaro Hiraide
- & Satoshi Watanabe
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| Open AccessReal-time signal processing via chemical reactions for a microfluidic molecular communication system
The use of electronic devices to process electrical signals in molecular communications can hardly realize its potential for various applications. Here, the authors report on chemical concentration signal processing in real time and digital signal transmission over distances.
- Vivien Walter
- , Dadi Bi
- & Yansha Deng
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Article
| Open AccessMg-incorporated sorbent for efficient removal of trace CO from H2 gas
The challenge of trace CO removal from H2 remains at the forefront of the hydrogen economy. Here, the authors demonstrated exceptional CO removal using a highly stable, hierarchically structured sorbent bead, Mg13CuCeOx. Mechanistic analysis showed the pivotal role of Mg in enhancing CO sorption.
- Gina Bang
- , Seongmin Jin
- & Chang-Ha Lee
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Article
| Open AccessPhotoelectric responsive ionic channel for sustainable energy harvesting
Artificial ion channels with multiple functions provide exciting opportunities to emulate natural processes and enhance energy conversion. Here, the authors introduce a family of photoelectrically responsive ionic covalent organic frameworks membranes for solar energy and salinity gradient energy conversion.
- Qing Guo
- , Zhuozhi Lai
- & Qi Sun
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| Open AccessEnergy-efficient extraction of linear alkanes from various isomers using structured metal-organic framework membrane
Extraction of linear alkanes from various isomers is critical for the petrochemical industry. Here authors present an oriented MOF membrane with a rigid triangular pore array for one-step extraction of linear pentane, hexane, and heptane from a ten-component alkane isomer solution.
- Yuecheng Wang
- , Yujie Ban
- & Weishen Yang
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Article
| Open AccessMaterial-agnostic machine learning approach enables high relative density in powder bed fusion products
Exploring laser powder bed fusion in manufacturing, the authors demonstrate a machine learning-based method to optimize processing conditions achieving materials with relative density greater than 98% and experimentally verify its generality for multiple distinct powder materials.
- Jaemin Wang
- , Sang Guk Jeong
- & Byeong-Joo Lee
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| Open AccessRationalizing kinetic behaviors of isolated boron sites catalyzed oxidative dehydrogenation of propane
The kinetic parameters in heterogeneous catalysis are informative in a mechanistic study. Here, the authors show the correlation between the coordination environment of isolated boron sites and the kinetics of oxidative dehydrogenation of propane.
- Hao Tian
- , Wenying Li
- & Bingjun Xu
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Article
| Open AccessTunable encapsulation of sessile droplets with solid and liquid shells
Encapsulated liquids are important for several microreactor applications, including (bio)chemistry in confined spaces. Here, the authors report on oil-infused particle shells that allow control of shell thickness, stability, and permeability for applications in crystal growth and cell cultivation.
- Rutvik Lathia
- , Satchit Nagpal
- & Prosenjit Sen
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Article
| Open AccessIntegrated urban water management by coupling iron salt production and application with biogas upgrading
Effective urban water management requires technological solutions that enable system-wide gains via a holistic approach. Here, authors propose an integrated system where an iron-oxidising electrochemical cell upgrades biogas while producing FeCO3 and subsequently uses the salt in wastewater treatment.
- Zhetai Hu
- , Lanqing Li
- & Zhiguo Yuan
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Article
| Open AccessDeposition and water repelling of temperature-responsive nanopesticides on leaves
Weak adhesion is a common hindrance to efficient utilization of pesticides in agricultural applications. Here, authors demonstrate leaf-adhesive tebuconazole nanopesticides which can be water-dispersed via flash nanoprecipitation using temperature-responsive copolymers PDMAEMA-b-PCL as the carrier.
- Jie Tang
- , Xiaojing Tong
- & Yisheng Xu
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Article
| Open AccessMechanism 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 AccessAn end-to-end pipeline for succinic acid production at an industrially relevant scale using Issatchenkia orientalis
Microbial production of succinic acid at an industrially relevant scale has been hindered by high downstream processing costs arising from neutral pH fermentation. Here, the authors report an end-to-end pipeline for succinic acid production at low pH using engineered acid-tolerant Issatchenkia orientalis strain.
- Vinh G. Tran
- , Somesh Mishra
- & Huimin Zhao
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| Open AccessThin lamellar films with enhanced mechanical properties for durable radiative cooling
Practical application of radiative cooling technology in harsh outdoor conditions remains challenging. Here, the authors develop a lamellar ANFs/Mica@TiO2 composite via a “solvent exchange-reprotonation” process enabling durable outdoor cooling.
- Lianhu Xiong
- , Yun Wei
- & Hua Deng
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Article
| Open AccessSolar-driven upgrading of biomass by coupled hydrogenation using in situ (photo)electrochemically generated H2
Green chemical transformations driven by renewable energies are imperative to realize a sustainable energy society. We demonstrate a coupled approach to hydrogenate biomass feedstock into valuable chemicals with high stability using hydrogen generated in situ in a (photo)electrochemical reactor.
- Keisuke Obata
- , Michael Schwarze
- & Fatwa F. Abdi
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Article
| Open AccessConcurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide
Electrosynthesis of hydrogen peroxide offers a cleaner, cost-effective alternative to anthraquinone processes. Here the authors report oxygen-deficient perovskite oxides with rich oxygen vacancies as bifunctional catalysts for concurrent oxygen reduction and water oxidation reactions in scalable hydrogen peroxide electrosynthesis.
- Changmin Kim
- , Sung O Park
- & Liming Dai
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Article
| Open AccessRegulating electrostatic phenomena by cationic polymer binder for scalable high-areal-capacity Li battery electrodes
Binders employed in battery electrodes are conventionally neutral linear polymers. Here, authors present a cationic semi-interpenetrating polymer network binder to regulate electrostatic phenomena, improving the properties and performance of high-capacity positive electrodes for Li metal batteries.
- Jung-Hui Kim
- , Kyung Min Lee
- & Sang-Young Lee
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Article
| Open AccessMethyl radical chemistry in non-oxidative methane activation over metal single sites
Understanding of the direct methane conversion mechanism is essential for further development of efficient catalysts. Here, authors demonstrate a general methyl radical chemistry for metal single site catalysis regardless of the support (either zeolite or SiO2) in non-oxidative methane activation.
- Xin Huang
- , Daniel Eggart
- & Xinhe Bao
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Article
| Open AccessA CO2 electrolyzer tandem cell system for CO2-CO co-feed valorization in a Ni-N-C/Cu-catalyzed reaction cascade
Tandem concepts for electroreduction of CO2 offer a valuable toolkit to tackle sluggish reaction kinetics and raise the production of e-chemicals. Here, the authors report a cascade system with two coupled electrolyzers using Ni-N-C and Cu-based catalysts for enhanced CO2 to multi-carbon conversion
- Tim Möller
- , Michael Filippi
- & Peter Strasser
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| Open AccessScalable electrosynthesis of commodity chemicals from biomass by suppressing non-Faradaic transformations
Electrooxidation of biomass provides a sustainable route to produce valuable chemicals, but suffers from non-Faradaic degradation in alkaline electrolysis at high reactant concentration. Here, the authors develop a single-pass continuous flow reactor to tackle this challenge, achieving kilogram-scale and continuous electrooxidation of glucose to formate and 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid with high selectivity and high concentration.
- Hua Zhou
- , Yue Ren
- & Haohong Duan
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| Open AccessMaximizing single-pass conversion does not result in practical readiness for CO2 reduction electrolyzers
The authors comment that maximizing product concentration is a more meaningful target for CO2 electrolyzers than maximizing single-pass conversion.
- Shashwati C. da Cunha
- & Joaquin Resasco
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Article
| Open AccessQuaternization-spiro design of chlorine-resistant and high-permeance lithium separation membranes
It is a current challenge to design chlorine-resistant polyamide lithium extraction nanofiltration membranes with high permeance. Here the authors address this challenge and produce large-area membranes by the interfacial polymerization of a quaternized-spiro piperazine monomer and trimesoyl.
- Huawen Peng
- , Kaicheng Yu
- & Qiang Zhao
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| Open AccessAdaptive multi-temperature control for transport and storage containers enabled by phase-change materials
Reliable transportation of multiple goods with different temperature requirements can logistically challenging. Here, the authors propose an adaptive multi-temperature control system using liquid-solid phase change materials to achieve effective thermal management using just a pair of heat and cold sources.
- Xinchen Zhou
- , Xiang Xu
- & Jiping Huang
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| Open AccessRegulating adsorption performance of zeolites by pre-activation in electric fields
The gas adsorption capacity and selectivity in zeolite molecular sieves can be regulated by an external electric field through the electric field-induced cation relocation and framework expansion.
- Kaifei Chen
- , Zhi Yu
- & Gang Kevin Li
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| Open AccessLarge-scale assembly of isotropic nanofiber aerogels based on columnar-equiaxed crystal transition
In this work, the authors present an ice-templating strategy to produce large-scale isotropic nanofiber aerogels using a unique process of freezing the material on a rotating cryogenic drum surface, crushing it, and then re-casting the nanofiber slurry enabling high-throughput and design flexibility.
- Lei Li
- , Yiqian Zhou
- & Hui Wu
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Article
| Open AccessSelf-adaptive amorphous CoOxCly electrocatalyst for sustainable chlorine evolution in acidic brine
Achieving stable and selective chlorine production is of high interest yet challenging. Here the authors report an amorphous CoOxCly catalyst prepared by in situ electrodeposition in acidic saline electrolyte which shows ~100% chlorine evolution selectivity with low overpotential and high stability over 500 h.
- Mengjun Xiao
- , Qianbao Wu
- & Chunhua Cui
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| Open AccessGuidelines for measuring and reporting particle removal efficiency in fibrous media
Adopting standardized and reliable methodologies to accurately measure particle removal efficiency when developing fibrous materials for controlling airborne contamination is crucial. Here, the authors recommend best practices for experimental assessments and reporting to ensure a reliable evaluation of new airborne particle filtration media and technologies.
- Paolo Tronville
- , Vincenzo Gentile
- & Jesus Marval
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Article
| Open AccessData-driven predictions of complex organic mixture permeation in polymer membranes
Membranes can be used for energy efficient organic liquid mixture separations. Here the authors use machine learning and transport simulations to predict the separation of complex mixtures such as crude oils by any linear polymer membrane.
- Young Joo Lee
- , Lihua Chen
- & Ryan P. Lively
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Article
| Open AccessNon-destructive erosive wear monitoring of multi-layer coatings using AI-enabled differential split ring resonator based system
Real-time monitoring of coatings erosive wear is critical to mitigate safety and financial concerns in many applications. Here, authors show a non-destructive inspection system with AI-enabled microwave resonators and a smart monitoring circuitry to identify and estimate wear depth and rate of eroded layers.
- Vishal Balasubramanian
- , Omid Niksan
- & Mohammad H. Zarifi
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Article
| Open AccessCoIn dual-atom catalyst for hydrogen peroxide production via oxygen reduction reaction in acid
The 2-electron oxygen reduction in acid is highly attractive to produce H2O2, a vital commodity chemical. Here, the authors report CoIn-N-C dual-atom catalyst for effective H2O2 production in acid, and show in-situ hydroxyl adsorption on In atoms is important for the selectivity alteration on nearby Co atoms.
- Jiannan Du
- , Guokang Han
- & Chunyu Du
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Article
| Open AccessSpying on parahydrogen-induced polarization transfer using a half-tesla benchtop MRI and hyperpolarized imaging enabled by automation
Hyperpolarized magnetic resonance imaging (MRI) has the potential to revolutionize MRI applications, but requires large and clumsy instruments. Here, the authors present a 0.5 T benchtop system that allows to hyperpolarize, image, and spy on nuclear spins like 13C within seconds.
- Frowin Ellermann
- , Aidan Sirbu
- & Andrey N. Pravdivtsev
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Article
| Open AccessIonomer-free and recyclable porous-transport electrode for high-performing proton-exchange-membrane water electrolysis
The supply of iridium is likely to become a bottleneck for hydrogen production. Here, authors develop ionomer-free porous transport electrodes with low iridium loading designed to improve manufacturability and recyclability of electrodes for proton exchange membrane water electrolyzers.
- Jason K. Lee
- , Grace Anderson
- & Xiong Peng
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Article
| Open AccessElectrosynthesis of ethylene glycol from C1 feedstocks in a flow electrolyzer
Ethylene glycol is an important commodity chemical and its production results in millions of tons of CO2 emissions annually. Here, the authors report a paired electrocatalytic strategy to produce ethylene glycol from methanol with a high Faradaic efficiency at industrial scale current density.
- Rong Xia
- , Ruoyu Wang
- & Feng Jiao
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Article
| Open AccessElucidating electrochemical nitrate and nitrite reduction over atomically-dispersed transition metal sites
Understanding of atomically dispersed metal-nitrogen-carbon (M-N-C) for electrochemical nitrate reduction is important and of high interest. Here, the authors employ a series of M-N-C catalysts to investigate selectivity correlation between nitrate and nitrite reduction.
- Eamonn Murphy
- , Yuanchao Liu
- & Plamen Atanassov
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Article
| Open AccessTuning the zeolite acidity enables selectivity control by suppressing ketene formation in lignin catalytic pyrolysis
Unveiling catalytic mechanisms at a molecular level aids selectivity control of lignin catalytic fast pyrolysis. Here authors show that the suppression of highly reactive ketenes is responsible for the five-fold phenol selectivity increase.
- Zeyou Pan
- , Allen Puente-Urbina
- & Patrick Hemberger