Featured
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| Open AccessDirect 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 AccessOn the role of asymmetric molecular geometry in high-performance organic solar cells
The correlation between asymmetric molecular geometry of non-fullerene acceptors and their optoelectronic properties was unclear. Here, the authors found asymmetric ones exhibit increased open-circuit voltage compared to their symmetric counterparts due to reduced non-radiative charge recombination.
- Jinfeng Huang
- , Tianyi Chen
- & Lijian Zuo
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Article
| Open AccessElectrocatalytic 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 AccessChlorine bridge bond-enabled binuclear copper complex for electrocatalyzing lithium–sulfur reactions
Here, the authors report a homonuclear cooper dual-atom electrocatalyst with high activity designed for synchronously boosting the sulfur and lithium evolutions.
- Qin Yang
- , Jinyan Cai
- & Yingze Song
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Article
| Open AccessEmbedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting
A robust and efficient dye-sensitized NiO bio-hybrid photocathode based on a redox polymer and [FeFe]- hydrogenase has been developed to couple with a BiVO4 photoanode for water splitting without applied bias.
- Fangwen Cheng
- , Olha Pavliuk
- & Haining Tian
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Article
| Open AccessEnhancing photocatalytic H2O2 production with Au co-catalysts through electronic structure modification
Photocatalytic H2O2 production using Au is hindered by its inherently weak O2 adsorption. Herein, the authors modify the electronic structure of Au with MoSx to form electron deficient Au sites to promote O2 adsorption and H2O2 production.
- Xidong Zhang
- , Duoduo Gao
- & Huogen Yu
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Article
| Open AccessMetavalently bonded tellurides: the essence of improved thermoelectric performance in elemental Te
Doping is a common strategy to improve thermoelectric performance yet limited to the solid solubility of dopants. Here, the authors find that forming metavalently bonded precipitates is key to property enhancement in Te rather than modifying the matrix lattice.
- Decheng An
- , Senhao Zhang
- & Yuan Yu
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Article
| Open AccessSolvent-free selective hydrogenation of nitroaromatics to azoxy compounds over Co single atoms decorated on Nb2O5 nanomeshes
Single atom catalysts can endow exceptional activity and selectively. Here, the authors report a single atom Co catalyst and reveal the importance of geometric and electronic properties for synthesizing azoxy compounds under solvent-free conditions.
- Zhijun Li
- , Xiaowen Lu
- & Yu Wang
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Article
| Open AccessPrecision 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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Article
| Open AccessThermally stable Ni foam-supported inverse CeAlOx/Ni ensemble as an active structured catalyst for CO2 hydrogenation to methane
An inverse CeAlOx/Ni/Ni-foam structured catalyst with high thermal stability and water resistance is shown to be effective at CO2 methanation across a wide temperature range because of efficient heat/mass transport.
- Xin Tang
- , Chuqiao Song
- & Lili Lin
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Article
| Open AccessManipulating the diffusion energy barrier at the lithium metal electrolyte interface for dendrite-free long-life batteries
Constructing an artificial solid electrolyte interphase to protect the lithium metal electrode is promising but challenging. Here, authors report a facile approach to form a layer to simultaneously overcome diffusion and advection-limited ion transport to achieve dendrite-free Li plating/stripping.
- Jyotshna Pokharel
- , Arthur Cresce
- & Yue Zhou
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Article
| Open AccessSurface oxidation/spin state determines oxygen evolution reaction activity of cobalt-based catalysts in acidic environment
Co-based catalysts are promising candidates for oxygen evolution reaction catalysis in an acidic environment, but the structure-activity relationship is unclear. Here, the authors discover that their acidic water oxidation activity is determined by the surface oxidation/spin state.
- Jinzhen Huang
- , Camelia Nicoleta Borca
- & Emiliana Fabbri
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Article
| Open AccessWater-assisted oxidative redispersion of Cu particles through formation of Cu hydroxide at room temperature
Redispersion of sintered metal species requires high temperatures in reactive atmospheres. Here, the authors report room temperature redispersion of supported Cu particles via formation of mobile hydroxylated Cu species induced by gaseous H2O and anchoring of the Cu species by surface OH groups.
- Yamei Fan
- , Rongtan Li
- & Qiang Fu
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Article
| Open AccessElectron paramagnetic resonance as a tool to determine the sodium charge storage mechanism of hard carbon
Hard carbons are considered the most suitable negative electrode materials for Na-ion batteries. Here, authors use electron paramagnetic resonance spectroscopy to determine the spin nature of mechanochemically-modified hard carbons to predict their charge storage mechanism for sodium-ion batteries.
- Bin Wang
- , Jack R. Fitzpatrick
- & Nuria Tapia-Ruiz
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Article
| Open AccessLigand-modified nanoparticle surfaces influence CO electroreduction selectivity
Enhancing the kinetics and selectivity of CO2/CO electroreduction towards valuable multi-carbon products poses a scientific challenge and is imperative for practical applicability. Here the authors report that modifying copper catalysts with surface thiol ligands significantly improves acetate selectivity.
- Erfan Shirzadi
- , Qiu Jin
- & Edward H. Sargent
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Article
| Open AccessOvercoming low initial coulombic efficiencies of Si anodes through prelithiation in all-solid-state batteries
All-solid-state batteries with silicon anodes have high capacities but low initial coulombic efficiencies (ICEs) because of first cycle irreversible capacity loss. Here, the authors report a prelithiation strategy to improve ICEs and reversibility.
- So-Yeon Ham
- , Elias Sebti
- & Ying Shirley Meng
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Article
| Open AccessA silicon photoanode protected with TiO2/stainless steel bilayer stack for solar seawater splitting
Here, the authors report a Si photoanode coated with a TiO2/stainless steel bilayer to inhibit chloride adsorption and facilitate stable alkaline seawater splitting for over 50 h with an applied bias photon-to-current efficiency of 2.62%.
- Shixuan Zhao
- , Bin Liu
- & Jinlong Gong
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Article
| Open AccessEfficient bubble/precipitate traffic enables stable seawater reduction electrocatalysis at industrial-level current densities
Seawater electroreduction is a promising technique for producing hydrogen, but it is hindered by cathodic Mg2 + /Ca2+ precipitation. Here, the authors propose a microscopic bubble/precipitate traffic system that releases small-sized bubbles across the cathode to repel Mg2 + /Ca2+ precipitates from almost the entire surface area of the catalyst.
- Jie Liang
- , Zhengwei Cai
- & Bo Tang
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Article
| Open AccessDiffusion-rate sieving of propylene and propane mixtures in a cooperatively dynamic porous crystal
Porous coordination polymers (PCPs) are commonly used in gas separation processes but developing PCPs that work at high temperatures and feature both high uptake capacity and selectivity remains challenging. Here, the authors report diffusion-rate sieving of propylene/propane at 300 K by constructing a PCP whose global and local dynamics cooperatively govern the adsorption process via gate opening for propylene and diffusion regulation for propane.
- Yan Su
- , Ken-ichi Otake
- & Cheng Gu
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Article
| Open AccessThe formation of unsaturated IrOx in SrIrO3 by cobalt-doping for acidic oxygen evolution reaction
SrIrO3-based catalyst is a promising candidate for acidic oxygen evolution reaction (OER), but the active sites and factors responsible for its effectiveness remain ambiguous. Here, the authors reveal that dynamic dissolution of Co in Co-SrIrO3 leads to the formation of unsaturated IrOx, enabling high-efficiency OER.
- Jia-Wei Zhao
- , Kaihang Yue
- & Gao-Ren Li
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Article
| Open AccessIsotope engineering achieved by local coordination design in Ti-Pd co-doped ZrCo-based alloys
Hydrogen isotope effect in metal-hydrogen systems disturbs precise Deuterium/Tritium (D/T) ratio control. Here, the authors demonstrate a local coordination strategy that comprises thermodynamic destabilization with vibration enhancement of interstitial isotopes for isotope engineering.
- Jiacheng Qi
- , Xu Huang
- & Lixin Chen
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Article
| Open AccessEnhancement of electrocatalysis through magnetic field effects on mass transport
Magnetic fields can enhance electrocatalysis, yet its effect on mass transport has been overlooked. Here, the authors track the motion induced on the electrolyte ions, demonstrating that mass transport effects can double the catalyst activity with low reactant availability, as in oxygen reduction.
- Priscila Vensaus
- , Yunchang Liang
- & Magalà Lingenfelder
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Article
| Open AccessJanus electronic state of supported iridium nanoclusters for sustainable alkaline water electrolysis
The hydrogen spillover effect improves the efficiency of the H2 evolution reaction but is incompatible with the O2 evolution reaction in alkaline water electrolysis. Here, the authors show that the Janus electronic state of supported Ir nanoclusters can couple hydrogen spillover and O2 evolution.
- Yaoda Liu
- , Lei Li
- & Zhengfei Dai
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Article
| Open AccessUltraviolet light blocking optically clear adhesives for foldable displays via highly efficient visible-light curing
The slow curing speed of UV-based methods to produce UV-blocking optically clear adhesive (OCA) for display panels poses a barrier to commercialization. Here, authors introduce a visible-light driven photo-initiating system for rapid production of OCAs, demonstrating efficient UV-blocking ability.
- Yonghwan Kwon
- , Seokju Lee
- & Min Sang Kwon
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Article
| Open AccessDefect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations
Converting nitrate to ammonia in wastewater with a wide range of nitrate concentrations remains a challenging task. Here the authors report defect-rich Cu nanowire electrocatalyst which can achieve 50 to 1100 mA cm−2 and over 90% Faradaic efficiency using 1–100 mM nitrate wastewater.
- Bocheng Zhang
- , Zechuan Dai
- & Genqiang Zhang
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Article
| Open AccessDeuteration-enhanced neutron contrasts to probe amorphous domain sizes in organic photovoltaic bulk heterojunction films
The use of conventional X-ray scattering techniques is challenging to detect donor-acceptor contrast within amorphous intermixing regions. Here, the authors apply neutron scattering and targeted deuteration to enhance the contrast by one order of magnitude and reveal short-range aggregations of d-Y6.
- Guilong Cai
- , Yuhao Li
- & Xinhui Lu
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Article
| Open AccessDynamical evolution of CO2 and H2O on garnet electrolyte elucidated by ambient pressure X-ray spectroscopies
Li6.5La3Zr1.5Ta0.5O12 (LLZO) is a promising solid electrolyte but suffers from severe surface degradation in air. Here, authors use mapping of resonant Auger spectroscopy and various ambient pressure X-ray spectroscopies to elucidate the dynamical evolution of CO2 and H2O on clean LLZO surfaces.
- Nian Zhang
- , Guoxi Ren
- & Xiaosong Liu
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Article
| Open AccessUltrastable halide perovskite CsPbBr3 photoanodes achieved with electrocatalytic glassy-carbon and boron-doped diamond sheets
Perovskites are desirable for photoelectrochemical applications but are unstable in aqueous electrolytes. Here, the authors report a perovskite photoanode in aqueous electrolyte, preserving 95% photocurrent density after over 100 h of operation.
- Zhonghui Zhu
- , Matyas Daboczi
- & Salvador Eslava
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Article
| Open AccessConstructing regulable supports via non-stoichiometric engineering to stabilize ruthenium nanoparticles for enhanced pH-universal water splitting
Establishing optimal metal-support interactions is crucial for creating efficient catalysts for water splitting. Here, stable Ti–O–Ru interface formation and minimal work function difference between Ru nanoparticles and non-stoichiometric Ti4O7 lead to exceptional bifunctional activity of Ru/Ti4O7 for both HER and OER across pH-universal environments, maintaining stable operation for 500 h.
- Sheng Zhao
- , Sung-Fu Hung
- & Shengjie Peng
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Article
| Open AccessHarnessing strong aromatic conjugation in low-dimensional perovskite heterojunctions for high-performance photovoltaic devices
The large organic cations in low-dimensional perovskite often introduces carrier mobility anisotropy and impedes charge transport. Here, authors report perovskite heterojunction with strong aromatic conjugated perovskites, realizing certified efficiency of over 25% in stable perovskite solar cells.
- Bo Li
- , Qi Liu
- & Zonglong Zhu
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Article
| Open AccessAn integrated high-throughput robotic platform and active learning approach for accelerated discovery of optimal electrolyte formulations
Solubility determines energy density in redox flow batteries. Here, authors combine automated experiments with machine learning to efficiently identify solvents that significantly enhance solubility, testing less than 10% of over 2000 candidates.
- Juran Noh
- , Hieu A. Doan
- & Yangang Liang
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Article
| Open AccessSynergistically optimized electron and phonon transport in high-performance copper sulfides thermoelectric materials via one-pot modulation
It is hard to simultaneously improve electrical and thermal properties of materials due to the strong coupling of carrier and phonon transport. Here, the authors propose a one-pot modulation strategy for simultaneously adjusting carrier and phonon transport in copper sulfids.
- Yi-Xin Zhang
- , Qin-Yuan Huang
- & Zhen-Hua Ge
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Article
| Open AccessSingle [0001]-oriented zinc metal anode enables sustainable zinc batteries
The authors present a single [0001]-oriented Zn metal anode with high reversibility and demonstrate the significance of the Zn(0002) metal anode, characterized by a single crystalline orientation, for promoting ultra-sustainable homoepitaxial growth.
- Xiaotan Zhang
- , Jiangxu Li
- & Jiang Zhou
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Article
| Open AccessUnderstanding 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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Article
| Open AccessCreation of flexible spin-caloritronic material with giant transverse thermoelectric conversion by nanostructure engineering
Nanostructure engineering enables transforming simple magnetic alloys into spincaloritronic materials with large transverse thermoelectric conversion. This has led to a high anomalous Nernst coefficient in flexible Fe-based amorphous alloys.
- Ravi Gautam
- , Takamasa Hirai
- & Hossein Sepehri-Amin
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Article
| Open AccessDecreasing exciton dissociation rates for reduced voltage losses in organic solar cells
The device’s electroluminescence efficiency is vital to reduce non-radiative voltage losses and boost organic solar cell performance. Here, the authors demonstrate that this efficiency is influenced not only by the decay of charge transfer states but also by the dissociation of singlet states.
- Hongbo Wu
- , Hao Lu
- & Zheng Tang
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Article
| Open AccessKeto-anthraquinone covalent organic framework for H2O2 photosynthesis with oxygen and alkaline water
Hydrogen peroxide photosynthesis is an important reaction that suffers from poor activity due to the high energy barrier of hydrogen extraction in water. Here, we report a keto-form anthraquinone framework that shows promising performance in alkaline conditions.
- Xiangcheng Zhang
- , Silian Cheng
- & Lizhi Zhang
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Article
| Open AccessSolar-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 AccessInduced dipole moments in amorphous ZnCdS catalysts facilitate photocatalytic H2 evolution
The rapid recombination of photogenerated charge carriers is a key challenge for photocatalytic hydrogen production. Here, the authors report an amorphous ZnCdS to break the symmetry of atom arrangement that induces strong dipole fields, thus providing extra driving forces for charge separation.
- Xin Wang
- , Boyan Liu
- & Songcan Wang
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Article
| Open AccessVacancies tailoring lattice anharmonicity of Zintl-type thermoelectrics
Vacancies are traditionally considered to play a role of phonon-defect scattering. Here, the authors show that vacancies can induce phonon softening, enhance phonon anharmonicity, and cause a dramatic reduction in the lattice thermal conductivity.
- Jinfeng Zhu
- , Qingyong Ren
- & Jie Ma
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Article
| Open AccessSpectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation
The authors report an in situ investigation of interfacial hydrogen spillover in Pd/ZIF-8 structures with X-ray and Raman techniques. A mechanistic picture of how Pd/ZIF-8 catalyst mediate alkyne semihydrogenation to alkynes is described.
- Qiaoxi Liu
- , Wenjie Xu
- & Yujie Xiong
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Article
| Open AccessStrain regulates the photovoltaic performance of thick-film perovskites
The power conversion efficiencies of thick-film perovskite solar cells lag behind those with nanometre film thickness. Here, the authors rule out the restrictions of carrier lifetime on device performance and reveal the critical role of lattice strain in micron-scale thick perovskite films.
- Pengju Shi
- , Jiazhe Xu
- & Rui Wang
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Article
| Open AccessAn entanglement association polymer electrolyte for Li-metal batteries
Here, the authors report an entanglement association polymer electrolyte with a polymer matrix and copolymer stabilizer. The developed entangled structure forms a stable interface for the polymer electrolyte during charging and discharging.
- Hangchao Wang
- , Yali Yang
- & Dingguo Xia
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Article
| Open AccessExtreme Li-Mg selectivity via precise ion size differentiation of polyamide membrane
Achieving high selectivity of Li+ and Mg2+ is of paramount importance for effective lithium extraction from brines, and nanofiltration (NF) membrane plays a critical role in this process. Here the authors report the fabrication of polyamide NF membranes with ultra-high Li + /Mg2+ selectivity by modifying the interfacial polymerization process with an oil-soluble surfactant.
- Quan Peng
- , Ruoyu Wang
- & Lei Jiang
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Article
| Open AccessA restricted dynamic surface self-reconstruction toward high-performance of direct seawater oxidation
Chlorine evolution reaction and deep reconstruction of catalyst are critical issues in direct seawater electrolysis. Here, the authors propose a MoO3/CoO/carbon composite material for improved selective seawater oxidation and restricted dynamic surface self-reconstruction.
- Ling Zhou
- , Daying Guo
- & Shun Wang
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Article
| Open AccessPulse potential mediated selectivity for the electrocatalytic oxidation of glycerol to glyceric acid
Mitigating the deactivation of noble metal-based catalysts caused by self-oxidation and toxic adsorption poses a considerable challenge in organic electro-oxidation. This study addresses the issue by employing a pulsed potential electrolysis approach to selectively electrocatalyze the oxidation of glycerol to glyceric acid using a Pt-based catalyst.
- Wei Chen
- , Liang Zhang
- & Yuqin Zou
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Article
| Open AccessPhenol as proton shuttle and buffer for lithium-mediated ammonia electrosynthesis
The proton shuttle plays a critical role in the proton transfer process during lithium-mediated ammonia synthesis. Here, the authors establish the structure-activity relationship and design principles for effective proton shuttles.
- Xianbiao Fu
- , Aoni Xu
- & Ib Chorkendorff
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Article
| Open AccessWell-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 AccessAssessing intra- and inter-molecular charge transfer excitations in non-fullerene acceptors using electroabsorption spectroscopy
The performance of Y6-containing donor-acceptor active layers in organic solar cells is highly related to the charge-transfer nature in Y6 aggregates. Here, authors study charge-transfer characteristics of excitations of isolated and aggregated Y6 molecules through electroabsorption spectroscopy.
- Sudhi Mahadevan
- , Taili Liu
- & Sai-Wing Tsang