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| Open AccessCO electrolysis to multicarbon products over grain boundary-rich Cu nanoparticles in membrane electrode assembly electrolyzers
Producing valuable chemicals like ethylene via catalytic CO conversion is an important nonpetroleum route. Here, authors demonstrate high-rate electrosynthesis of multicarbon chemicals via CO electrolysis, with a multicarbon product partial current density of 4.35 A cm−2 at a cell voltage of 2.78 V.
- Hefei Li
- , Pengfei Wei
- & Xinhe Bao
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Article
| Open AccessLow-temperature strain-free encapsulation for perovskite solar cells and modules passing multifaceted accelerated ageing tests
The instability of perovskite solar cells hinders their commercialization. Here, authors report an industrially compatible strain-free encapsulation process based on lamination of highly viscoelastic semi-solid/highly viscous liquid encapsulant adhesive to reduce thermomechanical interfacial stress.
- Paolo Mariani
- , Miguel Ángel Molina-García
- & Francesco Bonaccorso
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| Open AccessQuantum barriers engineering toward radiative and stable perovskite photovoltaic devices
Efficient radiation is essential to reach thermodynamic limit of photovoltaic efficiency. Here, authors design thick quantum barriers to suppress interfacial quenching and boost photon recycling in perovskite cells, achieving high radiation and photovoltaic efficiencies and long device stability.
- Kyung Mun Yeom
- , Changsoon Cho
- & Jun Hong Noh
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Article
| Open AccessThe impact of magnesium content on lithium-magnesium alloy electrode performance with argyrodite solid electrolyte
All-solid-state lithium-based batteries require high stack pressure during operation. Here, we investigate the mechanical, transport, and interfacial properties of Li-rich magnesium alloy and show enhanced performance at low pressure and ambient temperature for alloy-based electrodes with less than 5 at% Mg content.
- Jack Aspinall
- , Krishnakanth Sada
- & Mauro Pasta
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| Open AccessSynergetic regulation of SEI mechanics and crystallographic orientation for stable lithium metal pouch cells
The application of Li-metal batteries (LMBs) is impeded by unstable solid electrolyte interphase (SEI) and uncontrollable Li dendrites growth. Here, the authors present an YF3/PMMA composite layer to achieve high-performance LMBs via the synergetic regulation of SEI mechanics and Li crystallography.
- Yanhua Zhang
- , Rui Qiao
- & Jiangxuan Song
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Article
| Open AccessUnusual facet and co-catalyst effects in TiO2-based photocatalytic coupling of methane
Designing photocatalysts to enhance the efficiency of non-oxidative coupling of methane is a challenging task. Here, the authors report that the anatase TiO2 with exposed {101} facets and Pd co-catalyst enables efficient and selective methane coupling to ethane via a heterogeneous-homogeneous hybrid reaction pathway.
- Huizhen Zhang
- , Pengfei Sun
- & Ye Wang
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Article
| Open AccessReal-time observation of two distinctive non-thermalized hot electron dynamics at MXene/molecule interfaces
Photoexcited MXenes could transfer charge carriers to or heat molecules at their interfaces. Here, the authors show using time-resolved spectroscopy that the non-thermalized carriers can directly transfer to molecules or heat them within 125 fs.
- Qi Zhang
- , Wei Li
- & Xueming Yang
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Article
| Open AccessPd(II)/Pd(IV) redox shuttle to suppress vacancy defects at grain boundaries for efficient kesterite solar cells
Charge loss at grain boundaries of kesterite polycrystalline absorbers limits the performance of thin film solar cells. Here, authors report the use of Pd(II)/Pd(IV) redox shuttle to assist the capture and exchange of Se atoms and eliminate vacancy defects, realizing certified efficiency of 14.3%.
- Jinlin Wang
- , Jiangjian Shi
- & Qingbo Meng
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Article
| Open AccessLaCl3-based sodium halide solid electrolytes with high ionic conductivity for all-solid-state batteries
The advancement of sodium halide solid-state electrolytes can propel high-energy-density all-solid-state sodium-ion batteries. Here, the authors present a LaCl3-based electrolyte facilitating rapid Na+ ion conduction along the c-axis diffusion channel, ensuring high capacity even at elevated current densities.
- Chengyu Fu
- , Yifan Li
- & Hongfa Xiang
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Article
| Open AccessHighly reversible zinc metal anode enabled by strong Brønsted acid and hydrophobic interfacial chemistry
Trace amounts of strong acid can suppress Zn corrosion and promote uniform Zn deposition. Here, the authors use HTFSI to create a hydrophobic micro-environment at the Zn-electrolyte interface, enabling high efficiency and cycling stability.
- Qingshun Nian
- , Xuan Luo
- & Xiaodi Ren
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Article
| Open AccessPhysics-informed neural network for lithium-ion battery degradation stable modeling and prognosis
Reliable lithium-ion battery health assessment is vital for safety. Here, authors present a physics-informed neural network for accurate and stable state-of-health estimation, overcoming challenges of varied battery types and usage conditions.
- Fujin Wang
- , Zhi Zhai
- & Xuefeng Chen
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Article
| Open AccessAtomically dispersed Iridium on Mo2C as an efficient and stable alkaline hydrogen oxidation reaction catalyst
High-performance hydroxide exchange membrane fuel cells rely on the anode loading of platinum-group metals. Here, the authors report a highly active hydrogen oxidation electrocatalyst which contains atomically dispersed Ir on Mo2C nanoparticles supported on a carbon substrate.
- Jinjie Fang
- , Haiyong Wang
- & Zhongbin Zhuang
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Article
| Open AccessHigh-performance flexible p-type Ce-filled Fe3CoSb12 skutterudite thin film for medium-to-high-temperature applications
The authors fabricate p-type Fe3CoSb12-based skutterudite films exhibiting high thermoelectric performance, stability, and flexibility at medium-to-high temperatures, based on preparing custom target materials and pulsed laser deposition techniques.
- Dou Li
- , Xiao-Lei Shi
- & Zhi-Gang Chen
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Article
| Open AccessDivacancy and resonance level enables high thermoelectric performance in n-type SnSe polycrystals
N-type polycrystalline SnSe shows inferior ZT to p-type polycrystalline due to its high thermal conductivity and lower power factor. The authors overcome the problem via the synergy of divacancy defect and introducing resonance level into the conduction band.
- Yaru Gong
- , Wei Dou
- & Guodong Tang
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Article
| Open AccessPolyoxometalate-based plasmonic electron sponge membrane for nanofluidic osmotic energy conversion
Nanofluidic membranes have great potential in harvesting osmotic energy, but performance is hampered by insufficient permselectivity. Here, the authors solve this problem with a polyoxometalate-based nanofluidic plasmonic electron sponge membrane.
- Chengcheng Zhu
- , Li Xu
- & Chen Wang
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Article
| Open AccessA reactive neural network framework for water-loaded acidic zeolites
Modelling of acidic zeolites, one of the key industrial catalysts, under realistic operating conditions is currently limited to specific cases. Here, the authors report a machine learning framework allowing for accurate high-throughput modelling.
- Andreas Erlebach
- , Martin Šípka
- & Lukáš Grajciar
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Article
| Open AccessMonosymmetric Fe-N4 sites enabling durable proton exchange membrane fuel cell cathode by chemical vapor modification
The limited durability of metal-nitrogen-carbon electrocatalysts hinders their use in proton exchange membrane fuel cells for the oxygen reduction reaction. Here the authors transform active sites from FeN4 to stable monosymmetric FeN2 + N’2 via chemical vapor modification, resulting in enhanced improving the durability of the catalyst.
- Jingsen Bai
- , Tuo Zhao
- & Wei Xing
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Article
| Open AccessDisentangling the effects of structure and lone-pair electrons in the lattice dynamics of halide perovskites
By comparing CsSrBr3 and CsPbBr3 with close structural similarity but the latter lacking lone-pair electrons on the octahedral metal, the authors reveal the similar vibrational anharmonicities in the two perovskites, which disentangles the electronic properties and vibrational anharmonicities.
- Sebastián Caicedo-Dávila
- , Adi Cohen
- & David A. Egger
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| Open AccessSingle-zinc vacancy unlocks high-rate H2O2 electrosynthesis from mixed dioxygen beyond Le Chatelier principle
The principle of Le Chatelier is a fundamental concept in textbooks, serving as a guiding principle for controlling chemical and catalytic systems. In this study, the authors present an oxygen electroreduction system based on a single zinc vacancy catalyst, which operates in a manner that extends “beyond” Le Chatelier’s principle.
- Qi Huang
- , Baokai Xia
- & Sheng Chen
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| Open AccessSustainable upcycling of mixed spent cathodes to a high-voltage polyanionic cathode material
Direct recycling of critical battery materials bring promise but a challenge for the mixed cathode chemistries. Here, the authors report a sustainable upcycling approach, transforming degraded LiFePO4 and Mn-rich cathodes into a high-voltage polyanionic material with an increased energy density and economic value.
- Guanjun Ji
- , Di Tang
- & Hui-Ming Cheng
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Article
| Open AccessAtomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media
The relationship between the structural configurations of M-N-C electrocatalysts and their performances in neutral environments has been insufficiently investigated. Here the authors demonstrate that an ultralow metal-loaded Co-N-C electrocatalyst, featuring the asymmetric Co-C/N/O configuration, exhibit exceptional efficiency in electrochemically producing hydrogen peroxide under neutral conditions.
- Longxiang Liu
- , Liqun Kang
- & Guanjie He
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Article
| Open AccessSynergistic growth of nickel and platinum nanoparticles via exsolution and surface reaction
Utilizing “Chemistry at a point”, Ni is exsolved from a perovskite lattice under deposited Pt nanoparticles. This yields even smaller Ni Pt alloy nanoparticles on a perovskite nanofiber structure, exhibiting high catalytic activity.
- Min Xu
- , Yukwon Jeon
- & John T. S. Irvine
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| Open AccessThe roll-to-roll revolution to tackle the industrial leap for perovskite solar cells
Roll-to-Roll (R2R) coating is a technology that potentially enhances throughput, reduces costs, and accommodates flexible substrates for fabricating various types of solar cells and modules. Here, authors discuss the R2R revolution to tackle the industrial leap for perovskite photovoltaic devices.
- Ershad Parvazian
- & Trystan Watson
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Article
| Open AccessBicontinuous RuO2 nanoreactors for acidic water oxidation
Developing stable water oxidation catalysts is of great importance for proton-exchange membrane water electrolyzers. Here the authors report a bicontinuous nanoreactor composed of multiscale defected RuO2 nanocrystals for robust acidic water oxidation reactivity.
- Ding Chen
- , Ruohan Yu
- & Shichun Mu
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Article
| Open AccessLarge transverse thermoelectric effect induced by the mixed-dimensionality of Fermi surfaces
The conversion between longitudinal heat flow and transverse charge current is a promising energy harvesting technology. Here, the authors show the large transverse thermoelectric effect induced by the mixed-dimensionality of Fermi surfaces.
- Hikari Manako
- , Shoya Ohsumi
- & D. Aoki
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Article
| Open AccessA locally solvent-tethered polymer electrolyte for long-life lithium metal batteries
Solid polymer electrolytes containing N,N-dimethylformamide (DMF) exhibit improved Li+ conductivity but poor cycle life due to incompatibility between the Li metal anode and DMF. Here, the authors report a polymer electrolyte composited with Hofmann-DMF complex that achieves both high Li+ conductivity and long cycle life.
- Yanfei Zhu
- , Zhoujie Lao
- & Guangmin Zhou
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Article
| Open AccessCorrelating activities and defects in (photo)electrocatalysts using in-situ multi-modal microscopic imaging
Physicochemical heterogeneity poses a significant constraint in photocatalyst advancement. Here the authors introduce a multimodal optical microscopy platform to assess activity and defects concurrently in photoelectrocatalysts, revealing that disorder can unexpectedly enhance local photoelectrocatalytic performance in certain instances.
- Camilo A. Mesa
- , Michael Sachs
- & Raj Pandya
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Article
| Open AccessStarch-mediated colloidal chemistry for highly reversible zinc-based polyiodide redox flow batteries
The development of porous membranes that could work under high power density brings promise but a challenge with polyiodide cross-over for aqueous Zn-I flow batteries. Here, the authors develop a colloidal starch-based catholyte to inhibit cross-over that endows reversible flow cell performance.
- Zhiquan Wei
- , Zhaodong Huang
- & Chunyi Zhi
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Article
| Open AccessRealizing thermoelectric cooling and power generation in N-type PbS0.6Se0.4 via lattice plainification and interstitial doping
The authors fabricate a thermoelectric cooling device based on n-type PbS based material, which exhibits a remarkable cooling temperature difference of 36.9 K at room temperature, and the single-leg power generation efficiency of 8%.
- Lei Wang
- , Yi Wen
- & Li-Dong Zhao
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Article
| Open AccessPolymer hetero-electrolyte enabled solid-state 2.4-V Zn/Li hybrid batteries
Zn batteries suffer from low voltage due to the high redox potential of the Zn anode and the low potential of traditional cathodes. Here, the authors develop a polymer hetero-electrolyte, which allows separated Zn and Li reversibility and achieves a 2.4 V-Zn battery based on the LiNi0.5Mn1.5O4 cathode.
- Ze Chen
- , Tairan Wang
- & Chunyi Zhi
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Article
| Open AccessCreep-type all-solid-state cathode achieving long life
Electrochemical-mechanical issues bring challenges but create new opportunities to design innovative all-solid-state batteries. Here, the authors propose to use the (de)lithiation-stress-creep synergistic time-dependent evolution to boost the electrochemical performance of all-solid-state batteries.
- Xiaolin Xiong
- , Ting Lin
- & Liumin Suo
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Article
| Open AccessMolecular tuning boosts asymmetric C-C coupling for CO conversion to acetate
This work presents a general surface molecular tuning strategy to promote the electrochemical reduction of CO.
- Jie Ding
- , Fuhua Li
- & Bin Liu
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Article
| Open AccessSpatial decoupling of bromide-mediated process boosts propylene oxide electrosynthesis
The practical application of electrosynthesis of propylene oxide is hindered by limited performance. Here, the authors report a spatial decoupling strategy by utilizing the bromide mediator to link propylene and anode within separated reactors, realizing high-performance electrosynthesis of propylene oxide.
- Mingfang Chi
- , Jingwen Ke
- & Jie Zeng
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Article
| Open AccessEfficient tandem electroreduction of nitrate into ammonia through coupling Cu single atoms with adjacent Co3O4
An optimal catalyst for nitrate electroreduction should satisfy the simultaneously optimized adsorption of intermediates. Here, the authors report a tandem electrocatalyst by combining Cu single atoms with Co3O4 nanosheets, enhancing the binding with NO2−, thus promoting nitrate electroreduction to NH3.
- Yan Liu
- , Jie Wei
- & Jie Zeng
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| Open AccessNear-strain-free anode architecture enabled by interfacial diffusion creep for initial-anode-free quasi-solid-state batteries
Initially anode-free batteries with garnet-type solid-state electrolytes suffer from internal strain by repeated Li plating/stripping. Here, the authors propose a near-strain-free anode architecture for interfacial diffusion of Li metal that suppresses volume expansion during cycling.
- Kwang Hee Kim
- , Myung-Jin Lee
- & Jong Hyeok Park
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Article
| Open AccessConsummating ion desolvation in hard carbon anodes for reversible sodium storage
Hard carbon is regarded as a promising negative electrode for Na-ion batteries but suffers from low initial Coulombic efficiency (ICE). Here, the authors identify the time-dependent ion pre-desolvation on the nanopore of hard carbons, which remarkably improves the ICE by simply extending the aging time.
- Ziyang Lu
- , Huijun Yang
- & Haoshen Zhou
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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