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| Open AccessEfficient ammonia synthesis from the air using tandem non-thermal plasma and electrocatalysis at ambient conditions
The conversion of atmospheric N2 into NH3 under ambient pressure is highly interesting but very challenging. In this study, the authors present a tandem air-NOx and NOx-NH3 system that combines non-thermal plasma-enabled N2 oxidation with Ni(OH)x/Cu-catalyzed electrochemical NOx−reduction, resulting in a high NH3 yield from N2 under ambient pressure conditions.
- Wei Liu
- , Mengyang Xia
- & Guidong Yang
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Article
| Open AccessSub-millisecond lithiothermal synthesis of graphitic meso–microporous carbon
Porous carbons with high specific surface area and electronic conductivity are of interest for their electron and ion transport ability. Here authors use ultra-high temperature reactions of Li metal and polytetrafluoroethylene to make graphitized porous carbon for electrochemical energy storage.
- Huimin Zhang
- , Jingyi Qiu
- & Hao Zhang
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Article
| Open AccessBoosting thermoelectric performance of single-walled carbon nanotubes-based films through rational triple treatments
Authors introduce triple treatments to advance flexible single-walled carbon nanotube films, achieving a power factor of 20.29 µW cm−1 K−2. High structural stability and flexibility enable the fabrication of a high-power-density flexible device.
- Yuan-Meng Liu
- , Xiao-Lei Shi
- & Zhi-Gang Chen
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Article
| Open AccessHighly efficient anion exchange membrane water electrolyzers via chromium-doped amorphous electrocatalysts
Modulating the electronic structure of active metal sites is crucial to enhance the activity of anion-exchange membrane water electrolyzers. Here, the authors elaborate Cr-doped amorphous metal oxide catalysts with excellent activity and stability.
- Sicheng Li
- , Tong Liu
- & Tao Yao
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Article
| Open AccessLocal CO2 reservoir layer promotes rapid and selective electrochemical CO2 reduction
Converting CO2 to valuable chemicals is of high interest. Here the authors address the challenge of low CO2 solubility in water by incorporating a metal-organic framework layer to enhance CO2 pre-concentration and activation before its electroreduction by the underlying solid electrocatalyst.
- Subhabrata Mukhopadhyay
- , Muhammad Saad Naeem
- & Idan Hod
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Article
| Open AccessDouble cross-linked 3D layered PBI proton exchange membranes for stable fuel cell performance above 200 °C
Phosphoric acid (PA) doped proton exchange membranes (PEMs) often degrade above 200 °C due to membrane creeping, PA dehydration, and condensation. Here, the authors introduce gel-state polybenzimidazole PEMs with double cross-linked 3D layered structures, enabling efficient and stable fuel cell operation above 200 °C.
- Liang Zhang
- , Mengjiao Liu
- & Lixin Xue
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Article
| Open AccessUnderstanding the charge transfer effects of single atoms for boosting the performance of Na-S batteries
Efficient charge transfer in sulfur electrodes is a crucial challenge for sodium-sulfur batteries. Here, the authors developed a machine-learning-assisted approach to quickly identify effective single-atom catalysts that enhance selectivity for short-chain sodium polysulfides, leading to improved battery performance.
- Yao-Jie Lei
- , Xinxin Lu
- & Guoxiu Wang
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Article
| Open AccessGreen moisture-electric generator based on supramolecular hydrogel with tens of milliamp electricity toward practical applications
The emerging moisture-electric harvester suffers from insufficient power output. Here, the authors report a green, efficient, and scalable moisture-electric generator by introducing polyvinyl alcohol-sodium alginate hydrogel as active material.
- Su Yang
- , Lei Zhang
- & Xiaoming Tao
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Article
| Open AccessElectric-field-assisted proton coupling enhanced oxygen evolution reaction
Manganese complexes have long been utilized by nature to catalyze the oxygen evolution reaction (OER) but mirroring their efficiency in artificial electrochemical systems has proven difficult. This study centers on alpha-manganese dioxide (α-MnO2), which closely mimics natural MnIV-O-MnIII-HxO motifs, presenting a novel method for manipulating proton coupling within the OER process using an external electric field.
- Xuelei Pan
- , Mengyu Yan
- & Liqiang Mai
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Article
| Open AccessExtrinsic hydrophobicity-controlled silver nanoparticles as efficient and stable catalysts for CO2 electrolysis
A key factor for the electrochemical reduction of CO2 to CO is limiting the competing H2 evolution reaction. Here, authors use real-time synchrotron X-ray computed tomography to show that a silver nanoparticle-ligand catalyst structure improves water management, thereby maintaining CO production.
- Young-Jin Ko
- , Chulwan Lim
- & Hyung-Suk Oh
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Article
| 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
- & Magalí 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