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| Open AccessAtomic layer deposited Pt-Ru dual-metal dimers and identifying their active sites for hydrogen evolution reaction
Atomically precise control over elemental distributions presents a challenge in the preparation of catalytic nanomaterials. Here the authors report Pt-Ru bimetallic dimer structures through atomic layer deposition process and identify the roles of Pt and Ru in hydrogen evolution reaction.
- Lei Zhang
- , Rutong Si
- & Xueliang Sun
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Article
| Open AccessPrintable magnesium ion quasi-solid-state asymmetric supercapacitors for flexible solar-charging integrated units
Wearable self-powered electronics receive considerable attention, but development is hindered by bulky designs, energy storage systems, and safety issues. Here the authors demonstrate a flexible solar-charging integrated unit based on printed magnesium ion aqueous asymmetric supercapacitors.
- Zhengnan Tian
- , Xiaoling Tong
- & Zhongfan Liu
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Article
| Open AccessCollective excitation of plasmon-coupled Au-nanochain boosts photocatalytic hydrogen evolution of semiconductor
Plasmonic effect offers a valuable opportunity to improve the efficiency of semiconductor, photocatalysts. Here, the authors show that the collective excitation of plasmonic metal, nanoparticles is more favorable for enhancing the utilization of plasmonic energy by, semiconductors.
- Guiyang Yu
- , Jun Qian
- & Gang Liu
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| Open AccessThe rapid electrochemical activation of MoTe2 for the hydrogen evolution reaction
The performance of electrocatalysts for the renewable production of hydrogen is currently limited due to the difficulty of materials design. We show that tailoring the electronic structure under applied reductive bias is key to optimal electrocatalytic performance of a 2D chalcogenide material.
- Jessica C. McGlynn
- , Torben Dankwort
- & Alexey Y. Ganin
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| Open AccessAnomalous hydrogen evolution behavior in high-pH environment induced by locally generated hydronium ions
Most of the current understanding on electrocatalysis is obtained on bulk catalysts but has not been fully verified on nanostructured materials. An alternative alkaline hydrogen evolution reaction mechanism is proposed here for nanostructured catalysts.
- Xuesi Wang
- , Chaochen Xu
- & Shi-Zhang Qiao
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Article
| Open AccessPhotoinduced hydrogen release from hydrogen boride sheets
The development of lightweight and safe hydrogen carrier materials is desirable for hydrogen energy storage and release. Here, authors prepare hydrogen boride nanosheets and observe hydrogen gas production induced by light irradiation.
- Reiya Kawamura
- , Nguyen Thanh Cuong
- & Masahiro Miyauchi
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Article
| Open AccessThree-dimensional open nano-netcage electrocatalysts for efficient pH-universal overall water splitting
Water electrolysis is considered a key reaction for future sustainable fuel generation. Here, authors report a three-dimensional RuIrOx nano-netcage catalyst that shows high activities and efficiencies for pH-universal overall water splitting.
- Zewen Zhuang
- , Yu Wang
- & Yadong Li
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Article
| Open AccessSpecific ion effects at graphitic interfaces
Understanding aqueous solutions at graphitic interfaces is critical in a wide variety of emerging technologies. Here, the authors unravel specific ion effects at the interface with graphene and within graphene slit-pores by coupling first-principles simulations and electrochemical measurements.
- Cheng Zhan
- , Maira R. Cerón
- & Patrick G. Campbell
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Article
| Open AccessDynamic oxygen adsorption on single-atomic Ruthenium catalyst with high performance for acidic oxygen evolution reaction
Monitoring catalyst structural changes under working conditions is crucial for understanding how catalysts operate. Here, authors examine single-atom Ru electrocatalyst by operando synchrotron spectroscopies to identify the catalytic mechanism during the acidic oxygen evolution reaction.
- Linlin Cao
- , Qiquan Luo
- & Tao Yao
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Article
| Open AccessA general synthesis approach for amorphous noble metal nanosheets
While noble metal usage in catalysis is ubiquitous, the metals’ scarcity necessitates new materials designs for efficient utilization. Here, authors report a general strategy to prepare amorphous noble metal nanosheets and find the nanomaterials to act as efficient water-splitting electrocatalysts.
- Geng Wu
- , Xusheng Zheng
- & Yadong Li
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Article
| Open AccessSingle- and multi-component chiral supraparticles as modular enantioselective catalysts
Nanoscale biological assemblies play crucial roles in all living systems and display a variety of chemical functionalities. Here the authors show that it is possible to replicate some of the biochemical functions in similarly-sized assemblies made from inorganic nanoparticles.
- Si Li
- , Juan Liu
- & Nicholas A. Kotov
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Article
| Open AccessInterfacial oxygen vacancies yielding long-lived holes in hematite mesocrystal-based photoanodes
The performance of hematite (α-Fe2O3) photoanodes is limited by fast charge recombination. Here, authors develop hematite mesocrystal-based photoanodes with abundant interfacial oxygen vacancies for highly efficient solar water splitting under back illumination.
- Zhujun Zhang
- , Izuru Karimata
- & Takashi Tachikawa
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Article
| Open AccessDopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products
The electro-oxidative synthesis of valued chemicals offers to enhance the overall efficiency and economic viability of renewable electrosynthesis systems. Here, the authors use dopant-tuned catalysts to promote the electrosynthesis of dimethyl carbonate from CO and methanol via oxidative carbonylation.
- Tao-Tao Zhuang
- , Dae-Hyun Nam
- & Edward H. Sargent
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Article
| Open AccessNickel sulfide nanocrystals on nitrogen-doped porous carbon nanotubes with high-efficiency electrocatalysis for room-temperature sodium-sulfur batteries
Room temperature rechargeable sodium sulfur batteries are promising for next-generation energy storage systems, but their development is limited by polysulfide dissolution and slow kinetics. Here the authors report a cathode that serves as a multifunctional sulfur host and imparts enhanced performance.
- Zichao Yan
- , Jin Xiao
- & Shi-Xue Dou
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Article
| Open AccessUltrahigh β-phase content poly(vinylidene fluoride) with relaxor-like ferroelectricity for high energy density capacitors
Dielectric materials are candidates for electric high power density energy storage applications, but fabrication is challenging. Here the authors report a pressing-and-folding processing of a dielectric with relaxor-like behavior, leading to high energy density in a polymer-based dielectric capacitor.
- Nan Meng
- , Xintong Ren
- & Emiliano Bilotti
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Article
| Open AccessUtilizing solar energy to improve the oxygen evolution reaction kinetics in zinc–air battery
The authors here report a sunlight-promoted rechargeable zinc–air battery in which photoelectrode is used as the air electrode to substantially lower the charge potential under illumination. Notably, the battery can be initially charged with an extremely low voltage of ~1.20 V.
- Xiaorui Liu
- , Yifei Yuan
- & Wenbin Hu
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Article
| Open AccessCorrelation between manganese dissolution and dynamic phase stability in spinel-based lithium-ion battery
To unlock the potential of Mn-based cathode materials, the fast capacity fading process has to be first understood. Here the authors utilize advanced characterization techniques to look at a spinel LiMn2O4 system, revealing that a combination of irreversible structural transformations and Mn dissolution takes responsibility.
- Tongchao Liu
- , Alvin Dai
- & Khalil Amine
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Article
| Open AccessFast room temperature lability of aluminosilicate zeolites
While aluminosilicate zeolites are of interest for many applications, the affect of water on zeolite stability in mild aqueous conditions has yet to be established. Here, using ab initio calculations and NMR spectroscopy, the authors show that covalent bonds in the zeolite chabazite are labile when in contact with neutral liquid water.
- Christopher J. Heard
- , Lukas Grajciar
- & Russell E. Morris
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Article
| Open AccessBa-induced phase segregation and band gap reduction in mixed-halide inorganic perovskite solar cells
Element doping has been proven a useful strategy to tune the properties of halide perovskites. Here Xiang et al. show that barium unexpectedly does not incorporate in perovskite lattice but induces phase segregation and bandgap reduction and inhibits non-radiative recombination.
- Wanchun Xiang
- , Zaiwei Wang
- & Anders Hagfeldt
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| Open AccessAdvantages of eutectic alloys for creating catalysts in the realm of nanotechnology-enabled metallurgy
The combination of metallurgy concepts and nanotechnology with liquid metal processing has been largely unexplored. Here the authors use liquid-phase ultrasonication to produce a model system of catalytically active nano-alloys, demonstrating electrocatalysis and photocatalysis.
- Jianbo Tang
- , Rahman Daiyan
- & Kourosh Kalantar-Zadeh
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Article
| Open AccessReminiscent capillarity in subnanopores
Confined fluids in porous media exhibit different behaviors in large and small pores, the crossover between the two regimes being not well understood. Here the authors show, by experiments and simulations, that capillarity is reminiscent even for very small pore diameters, providing a unified picture.
- Irena Deroche
- , T. Jean Daou
- & Benoit Coasne
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Article
| Open AccessA universal ligand mediated method for large scale synthesis of transition metal single atom catalysts
Single-atom catalysts are a promising class of catalytic materials, but general synthetic methods are limited. Here, the authors develop a ligand-mediated strategy that allows the large-scale synthesis of diverse transition metal single atom catalysts supported on carbon.
- Hongzhou Yang
- , Lu Shang
- & Tierui Zhang
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| Open AccessUltrafast self-trapping of photoexcited carriers sets the upper limit on antimony trisulfide photovoltaic devices
Antimony trisulfide has a proper bandgap of 1.7 eV for making solar cells but the devices suffer from severe voltage loss. Here Yang et al. propose that the photoexcited carriers are self-trapped by lattice deformation, which places a thermodynamic limit of only 0.8 V for the open circuit voltage.
- Zhaoliang Yang
- , Xiaomin Wang
- & Haiming Zhu
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Article
| Open AccessAtomically ordered non-precious Co3Ta intermetallic nanoparticles as high-performance catalysts for hydrazine electrooxidation
Intermetallic nanoparticles comprised of early transition metals are attractive for fuel cell applications, but are generally limited to noble metal-based systems. Here, authors report non-precious early transition metal intermetallic nanoparticles with promising electrocatalytic performance for the hydrazine oxidation reaction.
- Guang Feng
- , Li An
- & Dingguo Xia
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Article
| Open AccessSynthesis of magnesium-nitrogen salts of polynitrogen anions
Polynitrogen compounds are potentially promising high energy density materials, but are difficult to synthesize due to their instability. Here, the authors observe the formation, under high pressure, of a Mg2N4 magnesium–tetranitrogen salt which remains stable at ambient conditions.
- Dominique Laniel
- , Bjoern Winkler
- & Natalia Dubrovinskaia
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| Open AccessEnhancing electron diffusion length in narrow-bandgap perovskites for efficient monolithic perovskite tandem solar cells
Tin-based perovskites possess the suitable narrow-bandgap for tandem solar cells but their short carrier diffusion lengths limit device efficiency. Here Yang et al. add cadmium ions to increase diffusion length to above 2 µm by reducing the background free hole concentration and electron trap density.
- Zhibin Yang
- , Zhenhua Yu
- & Jinsong Huang
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Article
| Open AccessZinc-doped Prussian blue enhances photothermal clearance of Staphylococcus aureus and promotes tissue repair in infected wounds
Here, the authors apply transition metal doping in combination with phototermal therapy to treat Staphylococcus aureus-infected wounds, and show that release of ions by local heat enhances bacteria clearance and promotes tissue repair in a rat model of MRSA-infected wounds
- Jun Li
- , Xiangmei Liu
- & Shuilin Wu
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Article
| Open AccessBottom-up growth of homogeneous Moiré superlattices in bismuth oxychloride spiral nanosheets
Expanding the range of available materials, methods for fabricating Moiré superlattices, and realization of new emergent properties are key challenges. Here the authors report a facile bottom-up synthesis of homogeneous Moiré superlattices based on a wide-gap 2D semiconductor, bismuth oxychloride.
- Lulu Liu
- , Yuanhui Sun
- & Weitao Zheng
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Article
| Open AccessIntegration of mesopores and crystal defects in metal-organic frameworks via templated electrosynthesis
Incorporating mesopores and active sites into metal-organic framework materials has proven advantageous for their catalytic application, but remains challenging to achieve. Here the authors obtain mesoporous, defect-rich metal-organic frameworks through templated electrosynthesis using ionic liquids as both electrolyte and template.
- Xinchen Kang
- , Kai Lyu
- & Martin Schröder
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| Open AccessLinking synthesis and structure descriptors from a large collection of synthetic records of zeolite materials
Understanding zeolite synthesis-structure relationships remains challenging owing to the number of variables involved in their preparation. Here the authors analyze zeolite synthetic records from the literature via machine learning and find communities of synthetically related materials with previously overlooked similarities.
- Koki Muraoka
- , Yuki Sada
- & Tatsuya Okubo
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Article
| Open AccessPhotocatalytic water splitting by N-TiO2 on MgO (111) with exceptional quantum efficiencies at elevated temperatures
Chemical fuels, produced from light, afford an alternative to fossil fuel, but conversion materials suffer from low photon-to-fuel efficiencies. Here, authors incorporate gold/N-doped TiO2 on MgO surfaces and show enhanced photocatalytic water splitting performances at elevated temperatures.
- Yiyang Li
- , Yung-Kang Peng
- & Shik Chi Edman Tsang
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Article
| Open AccessBoosting selective nitrogen reduction to ammonia on electron-deficient copper nanoparticles
Electrocatalytic nitrogen reduction is promising for ammonia production, but electrocatalysts are limited by low efficiency and high cost. Here, the authors report electron-deficient copper nanoparticles, induced by rectifying contact with polyimide, for selective reduction of nitrogen to ammonia.
- Yun-Xiao Lin
- , Shi-Nan Zhang
- & Jie-Sheng Chen
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Article
| Open AccessCarbon dioxide capture and efficient fixation in a dynamic porous coordination polymer
Porous coordination polymers that possess structural flexibility show great promise for gas adsorption and catalysis. Here the authors synthesize a dynamic porous coordination polymer with rotating ligands that permit effective CO2 trapping, and demonstrate subsequent CO2 cycloaddition to epoxides.
- Pengyan Wu
- , Yang Li
- & Susumu Kitagawa
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Article
| Open AccessUprooting defects to enable high-performance III–V optoelectronic devices on silicon
The use of promising group III-V materials for optoelectronic applications is hindered by the high density of threading dislocations when integrated with silicon technology. Here, the authors present an electrochemical deep etching strategy to drastically reduce the the defect density.
- Youcef A. Bioud
- , Abderraouf Boucherif
- & Richard Arès
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| Open AccessPerfect proton selectivity in ion transport through two-dimensional crystals
Defect-free monolayers of graphene and hexagonal boron nitride are highly permeable to thermal protons, but are impenetrable to gases. Here the authors show that mechanically exfoliated crystals exhibit perfect proton selectivity, corroborating proton transport through the bulk without atomic-scale defects.
- L. Mogg
- , S. Zhang
- & M. Lozada-Hidalgo
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Article
| Open AccessCross-linked beta alumina nanowires with compact gel polymer electrolyte coating for ultra-stable sodium metal battery
Here the authors show a beta alumina nanowires/gel polymer composite electrolyte design. The dense and homogeneous solid-liquid hybrid sodium-ion transportation channels promote uniform sodium deposition and stripping and significantly improve the performance of a Na metal battery.
- Danni Lei
- , Yan-Bing He
- & Feiyu Kang
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Article
| Open AccessCarrier lifetime enhancement in halide perovskite via remote epitaxy
Crystallographic dislocation has proven harmful to the carrier dynamics in conventional semiconductors but it is unexplored in metal halide perovskites. Here Jiang et al. grow remote epitaxial perovskite films on graphene with density-controlled dislocations and confirm their negative impact.
- Jie Jiang
- , Xin Sun
- & Jian Shi
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| Open AccessA high-performance oxygen evolution catalyst in neutral-pH for sunlight-driven CO2 reduction
Solar-to-fuel conversion under mild conditions offers a renewable means to store energy. Here authors report a Brownmillerite oxide for neutral-pH oxygen evolution that, when integrated with an anodized silver cathode, enables a 13.9% energy-conversion efficiency for light-driven CO2 reduction
- Li Qin Zhou
- , Chen Ling
- & Hongfei Jia
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Article
| Open AccessBalancing hydrogen adsorption/desorption by orbital modulation for efficient hydrogen evolution catalysis
Hydrogen adsorption/desorption behavior plays a key role in hydrogen evolution reaction catalysis. Here, the authors demonstrate the rational balancing of hydrogen adsorption/desorption by orbital modulation for significantly enhanced hydrogen evolution performance.
- Feng Li
- , Gao-Feng Han
- & Jong-Beom Baek
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Article
| Open AccessDirect evidence for grain boundary passivation in Cu(In,Ga)Se2 solar cells through alkali-fluoride post-deposition treatments
Grain boundaries play critical roles in determining the properties and performance of solar cells based on polycrystalline materials. Here Nicoara et al. showcase that proper treatments passivate defects at grain boundaries by forming secondary material phases with the CIGSe absorbers and lead to higher Voc.
- Nicoleta Nicoara
- , Roby Manaligod
- & Sascha Sadewasser
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Article
| Open AccessTriggered reversible phase transformation between layered and spinel structure in manganese-based layered compounds
The irreversible layered-to-spinel phase transformation is detrimental for many cathode materials. Here, the authors show that reversibility can be realized in crystal water containing sodium birnessite by controlled dehydration, leading to enhanced ion diffusion kinetics and improved structural stability.
- Mi Ru Jo
- , Yunok Kim
- & Yong-Mook Kang
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Article
| Open AccessAtomic and electronic modulation of self-supported nickel-vanadium layered double hydroxide to accelerate water splitting kinetics
While water-splitting affords a renewable means to store energy, expensive catalysts are often required to achieve high performances. Here, authors modulate nickel-vanadium double hydroxide properties by noble-metal doping to accelerate electrocatalytic water splitting kinetics.
- Dewen Wang
- , Qun Li
- & Xiurong Yang
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Article
| Open AccessMolecular cobalt corrole complex for the heterogeneous electrocatalytic reduction of carbon dioxide
Electrochemical conversion of carbon dioxide to ethanol is one of the most challenging energy conversion reactions. Here the authors show selective electroreduction of carbon dioxide to ethanol by using a functionalized cobalt A3-corrole catalyst immobilized on a carbon paper electrode.
- Sabrina Gonglach
- , Shounik Paul
- & Soumyajit Roy
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Article
| Open AccessAtomistic structures and dynamics of prenucleation clusters in MOF-2 and MOF-5 syntheses
Numerous techniques have been used to study the crystallization process of metal-organic frameworks, but little is known about their prenucleation clusters. Here the authors use single-molecule atomic-resolution real-time electron microscopic video imaging to identify prenucleation clusters in the synthesis of MOF-2 and MOF-5.
- Junfei Xing
- , Luca Schweighauser
- & Eiichi Nakamura
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Article
| Open AccessQuadruple perovskite ruthenate as a highly efficient catalyst for acidic water oxidation
Electrocatalytic water splitting provides a renewable path to store energy in chemical bonds, but highly efficient oxygen-evolving catalysts in acid media remain limited. Here the authors report a quadruple perovskite ruthenate oxide as an effective and stable oxygen evolution electrocatalyst.
- Xianbing Miao
- , Lifu Zhang
- & Shiming Zhou
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Article
| Open AccessScreening highly active perovskites for hydrogen-evolving reaction via unifying ionic electronegativity descriptor
Facile and reliable screening of efficient electrocatalysts is important for energy conversion technologies such as water splitting. Here, authors introduce A-site ionic electronegativity as a descriptor to understand the hydrogen-evolution activities of cobalt-based perovskites.
- Daqin Guan
- , Jing Zhou
- & Zongping Shao
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Article
| Open AccessTuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts
Converting solar energy to hydrogen fuel requires light-absorbers that well-match the wavelengths of incoming sunlight. Here, authors prepare a broadband visible-light-absorbing molecular complex that efficiently produces hydrogen from water.
- Ji Hoon Lee
- , Shyam Kattel
- & Jingguang G. Chen
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Article
| Open AccessDirectly transforming copper (I) oxide bulk into isolated single-atom copper sites catalyst through gas-transport approach
Single-atom catalysts attract lots of attention, but direct transformation of bulk metal oxide into single atoms remains challenging. Here the authors report a gas-transport route to transform monolithic copper (I) oxide into copper single-atoms catalyst with a high activity for oxygen reduction.
- Zhengkun Yang
- , Bingxu Chen
- & Yuen Wu
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Article
| Open AccessStrong light-matter coupling for reduced photon energy losses in organic photovoltaics
Strong light-matter coupling can tune exciton properties but its effect in photovoltaics remains unexplored. Here Nikolis et al. show that the photon energy loss from optical gap to open-circuit voltage can be reduced to unprecedented values by embedding organic solar cells in optical microcavities.
- Vasileios C. Nikolis
- , Andreas Mischok
- & Koen Vandewal