Featured
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Article
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Direct conversion of methane to aromatics and hydrogen via a heterogeneous trimetallic synergistic catalyst
Converting methane to hydrogen and aromatics is a route to upgrading natural gas into high value products. Here the authors report a high-performing synergistic trimetallic thermochemical catalyst, along with mechanistic insights into the process.
- Pengxi Zhu
- , Wenjuan Bian
- & Hanping Ding
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Article
| Open Access
Electrocatalytic hydrogenation of acetonitrile to ethylamine in acid
Proton exchange membrane electrolyzers hold promise for ethylamine synthesis from acetonitrile, yet local acidity fosters proton reduction. Here, authors systematically screen metal catalysts, verifying their effectiveness in such electrolyzers.
- Chongyang Tang
- , Cong Wei
- & Xiangfeng Duan
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Article
| Open Access
Precision ion separation via self-assembled channels
Selective nanofiltration membranes with accurate molecular sieving offer a solution to recover rare metals and other valuable elements from brines but this demands the development of membranes with precise sub-nanometer pores surpassing those available today. Here, the authors report a scalable approach for membrane fabrication in which functionalized macrocycles are seamlessly oriented via supramolecular interactions during the interfacial polycondensation on a polyacrylonitrile support layer.
- Shanshan Hong
- , Maria Di Vincenzo
- & Suzana P. Nunes
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| Open Access
Reverse water gas-shift reaction product driven dynamic activation of molybdenum nitride catalyst surface
Catalyst activation commonly occurs during reactions. This study demonstrates that the surface’s active structure in nitride catalysts during the reverse water gas-shift reaction varies with the partial pressure of reaction products, resulting in enhanced catalytic activity through positive feedback between catalytic activity and the evolution of MoNx’s active structure.
- Hui Xin
- , Rongtan Li
- & Xinhe Bao
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| Open Access
Low-nuclearity CuZn ensembles on ZnZrOx catalyze methanol synthesis from CO2
The ideal metal selection and atomic-level arrangement for catalysts in CO2 hydrogenation are still uncertain. Here, copper is identified as the most effective promoter for enhancing ZnZrOx catalysts when precisely structured into CuZn ensembles, offering new insights for designing superior catalysts for CO2-based methanol synthesis.
- Thaylan Pinheiro Araújo
- , Georgios Giannakakis
- & Javier Pérez-Ramírez
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| Open Access
Transparent ultrahigh-molecular-weight polyethylene/MXene films with efficient UV-absorption for thermal management
While MXene-based composites have been reported as promising materials for photothermal conversion, their opaque appearance limits applications. Here, authors demonstrate visible-light transparent and UV-absorbing composite films by vacuum pressing solution blends of MXene with polyethylene.
- Xianhu Liu
- , Wenrui Zhang
- & Changyu Shen
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Article
| Open Access
Upgrading CO2 to sustainable aromatics via perovskite-mediated tandem catalysis
The transformation of CO2 with renewable hydrogen into high-value products presents a sustainable route for net-zero chemical manufacture. Here the authors introduce a LaFeO3 perovskite-mediated tandem conversion of CO2, achieving remarkable performance by separating the CO2 hydrogenation and C-C coupling domains in the catalyst system.
- Guo Tian
- , Zhengwen Li
- & Fei Wei
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| Open Access
Ultrathin organosiloxane membrane for precision organic solvent nanofiltration
The use of membranes under harsh conditions, particularly involving the separation of complex organic solvents, remains challenging. Here the authors demonstrate an ultrathin organosiloxane polymer membrane using initiated chemical vapor deposition to effectively separate solutes within the molecular weight range of 150–300 g mol−1.
- Jihoon Choi
- , Keonwoo Choi
- & Dong-Yeun Koh
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| Open Access
Understanding the effect of spatially separated Cu and acid sites in zeolite catalysts on oxidation of methane
Methane is a potent greenhouse gas, and its removal is critical. Here, the authors demonstrate that spatially separated Cu and acid sites in Cu/zeolites influence product distribution and efficiency for methane oxidation.
- Peipei Xiao
- , Yong Wang
- & Toshiyuki Yokoi
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| Open Access
Predicting and improving complex beer flavor through machine learning
Perception and appreciation of food flavour depends on many factors, posing a challenge for effective prediction. Here, the authors combine extensive chemical and sensory analyses of 250 commercial Belgian beers to train machine learning models that enable flavour and consumer appreciation prediction.
- Michiel Schreurs
- , Supinya Piampongsant
- & Kevin J. Verstrepen
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Article
| Open Access
Solar-driven sugar production directly from CO2 via a customizable electrocatalytic–biocatalytic flow system
Solar-driven artificial food synthesis from CO2 provides an approach to overcome the limitations of natural photosynthesis, but it is very challenging. Here, the authors report a hybrid electrocatalytic-biocatalytic flow system, coupling photovoltaics-powered electrocatalysis (CO2 to formate) with a five enzyme cascade platform (formate to sugar), which achieves conversion of CO2 to C6 sugar (L-sorbose) with a solar-to-food energy conversion efficiency of 3.5%.
- Guangyu Liu
- , Yuan Zhong
- & Yujie Xiong
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Article
| Open Access
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
Strategies for high-temperature methyl iodide capture in azolate-based metal-organic frameworks
Efficient capture of methyl iodide (CH3I) from high-temperature nuclear off-gas is quite challenging. Here, the authors present two innovative and efficient strategies to adsorb CH3I at high temperatures in an azolate-based metal-organic framework.
- Tingting Pan
- , Kaijie Yang
- & Yu Han
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| Open Access
Supra-biological performance of immobilized enzymes enabled by chaperone-like specific non-covalent interactions
Designing complex synthetic materials for enzyme immobilization could unlock the utility of biocatalysis in extreme environments. Here, the authors report on random copolymer brushes as dynamic immobilization supports that enable supra-biological catalytic performance of immobilized enzymes.
- Héctor Sánchez-Morán
- , Joel L. Kaar
- & Daniel K. Schwartz
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Article
| Open Access
Double charge flips of polyamide membrane by ionic liquid-decoupled bulk and interfacial diffusion for on-demand nanofiltration
Currently polyamide membranes fabricated by interfacial polymerization are limited by inherently negative charge as well as narrow charge tailoring window restricting the application of these membranes. Here, the authors report a facile ionic liquid-decoupled bulk/interfacial diffusion strategy to fabricate polyamide membranes which can transform on-demand from inherently negative to highly positive and near-neutral charge.
- Bian-Bian Guo
- , Chang Liu
- & Zhi-Kang Xu
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| Open Access
The first demonstration of entirely roll-to-roll fabricated perovskite solar cell modules under ambient room conditions
The translation of perovskite solar cells to large-area devices fabricated by industry-relevant manufacturing methods remains a critical challenge. Here, authors report solar modules with serially-interconnected cells produced entirely by industrial roll-to-roll printing under ambient conditions.
- Hasitha C. Weerasinghe
- , Nasiruddin Macadam
- & Doojin Vak
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| 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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| Open Access
Copper nanoparticles encapsulated in zeolitic imidazolate framework-8 as a stable and selective CO2 hydrogenation catalyst
Here, authors report an inter-site structural heterogeneity induced effect of hierarchical single atom Fe catalysts for robust oxygen reduction. Dynamic evolutions and insights into structure-activity relationship are presented.
- Vijay K. Velisoju
- , Jose L. Cerrillo
- & Pedro Castaño
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| Open Access
Understanding activity-stability tradeoffs in biocatalysts by enzyme proximity sequencing
Understanding the complex relationships between enzyme sequence, folding stability and catalytic activity is essential for applications, but current technologies cannot simultaneously resolve both stability and activity phenotypes and couple these to gene sequences at large scale. Here, the authors report Enzyme Proximity Sequencing (EP-Seq), a deep mutational scanning method to assay both expression level and catalytic activity of thousands of oxidoreductase variants from a cellular pool in a single experiment.
- Rosario Vanella
- , Christoph Küng
- & Michael A. Nash
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| Open Access
Moiré effect enables versatile design of topological defects in nematic liquid crystals
Precise manipulation and utilization of the topological structures in liquid crystals remain challenging tasks. Wang et al. use the moiré effect combined with surface patterning to create highly tunable, arbitrary topological defects.
- Xinyu Wang
- , Jinghua Jiang
- & Rui Zhang
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| Open Access
Ultrathin, ultralight dual-scale fibrous networks with high-infrared transmittance for high-performance, comfortable and sustainable PM0.3 filter
Development of high-performance, comfortable and sustainable air filters is challenging. Here, authors design an ultrathin, ultralight dual scale fiber mat composed of true nanofibers and submicron-fibers to integrate the high protection, thermal wet comfort and save raw materials.
- Yuchen Yang
- , Xiangshun Li
- & Yuekun Lai
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| Open Access
Tuning ferroelectric phase transition temperature by enantiomer fraction
The enantiomer fraction strategy can achieve continuous control of the phase transition temperature, chiroptical properties, SHG intensity and other properties of chiral two-dimensional lead bromide ferroelectrics.
- Chang-Chun Fan
- , Cheng-Dong Liu
- & Wen Zhang
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| Open Access
Chiral active particles are sensitive reporters to environmental geometry
There hasn’t been much experimental attention to the interaction of chiral active particles with complex environments. Chan et al. propose an interesting granular particle system based on natural plant seeds to examine the transport of chiral active matter in complex surroundings.
- Chung Wing Chan
- , Daihui Wu
- & Rui Zhang
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Perspective
| Open Access
Performance metrics to unleash the power of self-driving labs in chemistry and materials science
Assessing the performance of self-driving labs (SDLs) is challenging due to the specificities of each experiment. In this Perspective, the authors review recent literature of SDLs for materials science and chemistry and suggest how to report SDL performance more effectively.
- Amanda A. Volk
- & Milad Abolhasani
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Article
| Open Access
Biomimetic mercury immobilization by selenium functionalized polyphenylene sulfide fabric
The abatement of elemental mercury remains an enormous challenge for public health and ecosystems. Here, inspired by the seleno-mercury antagonism effect in biological systems, the authors developed an ideal Hg0 adsorbent with a record-high adsorption capacity of 1621.9 mg g−1.
- Hailong Li
- , Fanyue Meng
- & Jianping Yang
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Article
| Open Access
An integrated self-optimizing programmable chemical synthesis and reaction engine
A limitation of robotic platforms in chemistry is the lack of feedback loops to adjust the conditions in-operando. Here the authors present a dynamically programmable robotic system that uses sensors for real-time adaptation, achieving yield improvements in syntheses and discovering new molecules.
- Artem I. Leonov
- , Alexander J. S. Hammer
- & Leroy Cronin
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Article
| Open Access
Re-evaluation of battery-grade lithium purity toward sustainable batteries
Due to recent fluctuations in lithium prices, the instability of lithium-ion batteries prices is on the rise. Here, through a re-evaluation of purity criteria, the authors report that the presence of magnesium impurity in lithium precursor actually improves cathode performance, economics, and environmental aspects.
- Gogwon Choe
- , Hyungsub Kim
- & Yong-Tae Kim
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Article
| Open Access
Visualization-enhanced under-oil open microfluidic system for in situ characterization of multi-phase chemical reactions
Under-oil open microfluidic systems have potential for studying multi-phase chemical reactions but have so far demonstrated largely only for biological applications. Here, the authors report the development of a system for in situ characterization of gas-liquid reactions by Raman spectroscopy.
- Qiyuan Chen
- , Hang Zhai
- & Bu Wang
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| Open Access
Challenging thermodynamics: combining immiscible elements in a single-phase nano-ceramic
Elemental immiscibility limits the development of solid solution materials. Here, authors create a nonequilibrium flame aerosol method to mix nearly any pair of metal elements in a single-phase nano-ceramic. Also, an exsolution behavior is presented to produce active and stable nanoparticles.
- Shuo Liu
- , Chaochao Dun
- & Mark T. Swihart
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Article
| Open Access
Interplay of the forces governing steroid hormone micropollutant adsorption in vertically-aligned carbon nanotube membrane nanopores
Micropollutant removal in polymeric nanofiltration membranes is difficult to characterise due to pore heterogeneity. A force interplay framework was developed to describe adsorption in VaCNT membranes with defined nanopores, providing insight for the design of membranes with improved selectivity.
- Minh N. Nguyen
- , Melinda L. Jue
- & Andrea I. Schäfer
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Article
| Open Access
Development of multifunctional membranes via plasma-assisted nonsolvent induced phase separation
The structures and properties of membranes depend strongly on their preparation methods. Here, the authors present a plasma-assisted nonsolvent-induced phase separation method that allows to tailor the physicochemical and electrical characteristics of PVDF membranes for various applications.
- Yueh-Han Huang
- , Meng-Jiy Wang
- & Tai-Shung Chung
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Article
| Open Access
Printed smart devices for anti-counterfeiting allowing precise identification with household equipment
The authors introduce a flexible laser printing method for synthesizing integrated optical and electric Physical Unclonable Functions (PUFs). The PUF devices can be read out by simple household equipment and show high uniqueness and stability.
- Junfang Zhang
- , Rong Tan
- & Felix F. Loeffler
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Article
| Open Access
Unraveling the rate-determining step of C2+ products during electrochemical CO reduction
The electrochemical reduction of CO for sustainable fuel production has gained attention, but the reaction mechanism needs further clarification. Here the authors delve into the discussion regarding whether the rate-determining step for the generation of multi-carbon products is the C-C coupling or the hydrogenation of CO, and provide evidence for dimerization of two *CO as the pivotal step in this process.
- Wanyu Deng
- , Peng Zhang
- & Jinlong Gong
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| Open Access
Efficient conversion of propane in a microchannel reactor at ambient conditions
The activation of propane at mild conditions is challenging. Now a microfluidic reaction system with a Cu microtube serving as both the catalyst and the microchannel reactor can selectively convert propane to propylene at room temperature and ambient pressure.
- Chunsong Li
- , Haochen Zhang
- & Qi Lu
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| Open Access
Catalytic carbon–carbon bond cleavage in lignin via manganese–zirconium-mediated autoxidation
Efforts to produce aromatic monomers through catalytic lignin depolymerization were focused on aryl–ether bond cleavage, while the carbon–carbon bonds of a large fraction of aromatic monomers in lignin are difficult to cleave. Here, the authors report a catalytic autoxidation method using manganese and zirconium salts as catalysts to cleave the C–C bonds in lignin-derived dimers and oligomers from pine and poplar.
- Chad T. Palumbo
- , Nina X. Gu
- & Gregg T. Beckham
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Article
| Open Access
Aqueous amine enables sustainable monosaccharide, monophenol, and pyridine base coproduction in lignocellulosic biorefineries
Utilization of the entire lignocellulose is essential for sustainable and cost-effective biorefineries, but it is hindered by a trade-off between efficient carbohydrate utilization and lignin-to-chemical conversion yield. Here, the authors report a mild lignocellulosic fractionation process using aqueous diethylamine which produces a carbohydrate fraction susceptible to enzymatic hydrolysis and a high-quality lignin that delivers high monomer yields upon catalytic amination and depolymerization.
- Li Xu
- , Meifang Cao
- & Xueqing Qiu
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Article
| Open Access
A dynamic knowledge graph approach to distributed self-driving laboratories
Global challenges demand global solutions. Here, the authors show a distributed self-driving lab architecture in The World Avatar, linking robots in Cambridge and Singapore for asynchronous multi-objective reaction optimisation.
- Jiaru Bai
- , Sebastian Mosbach
- & Markus Kraft
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Article
| Open Access
Interaction-selective molecular sieving adsorbent for direct separation of ethylene from senary C2-C4 olefin/paraffin mixture
Olefin/paraffin separations are challenging in chemical industry. Here, authors report a sieving adsorbent for separating C2-C4 olefins from counterpart paraffins. The interlayer spaces are selectively opened via stronger guest-host interactions induced by olefins, as opposed to saturated paraffins.
- Yong Peng
- , Hanting Xiong
- & Jun Wang
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Article
| Open Access
CO2 hydrogenation over Fe-Co bimetallic catalysts with tunable selectivity through a graphene fencing approach
Product-selective switching of CO2 hydrogenation is a huge challenge. Here, the authors report an approach to manipulating Fe-Co sites with three-dimensional graphene fences that achieves integrated synthesis of different products.
- Jiaming Liang
- , Jiangtao Liu
- & Noritatsu Tsubaki
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Article
| Open Access
A micro-architectured material as a pressure vessel for green mobility
A shellular is a micro-architectured material, composed of a continuous smooth-curved thin shell in the form of a triply periodic minimal surface. Here, authors propose schellular designs applied to pressure vessels and demonstrate its competitive practical features against spherical and cylindrical vessels.
- Yoon Chang Jeong
- , Seung Chul Han
- & Kiju Kang
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Article
| Open Access
Reprogramming 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 Access
Nanowire-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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Article
| Open Access
Organohydrogel-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 Access
Roll-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 Access
PolyMOF 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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| Open Access
Enhanced 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 Access
Enabling 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 Access
Design 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 Access
Programmable 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
Nanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation