Featured
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Article
| Open AccessMechanistic insights into CO2 conversion chemistry of copper bis-(terpyridine) molecular electrocatalyst using accessible operando spectrochemistry
Transition metal complexes are potential low-cost electrocatalysts for CO2 reduction. Here, using accessible spectrochemistry, the authors observe an intriguing baton relay-like mechanism of active site transfer during CO2 reduction to CO on a carbon-supported copper bis-(terpyridine) complex.
- Huihui Zhang
- , Chang Xu
- & Yi Xie
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Article
| Open AccessBias-free solar hydrogen production at 19.8 mA cm−2 using perovskite photocathode and lignocellulosic biomass
While light-driven water splitting offers a means to produce renewable H2 fuel, water oxidation limits performances and yields low-value products. Here, authors demonstrate a photoelectrochemical cell that converts lignocellulosic biomass into valuable products alongside H2.
- Yuri Choi
- , Rashmi Mehrotra
- & Jungki Ryu
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Article
| Open AccessInterface engineering breaks both stability and activity limits of RuO2 for sustainable water oxidation
RuO2 encounters critical electrochemical dissolution issues during oxygen evolution reaction and it remains a grand challenge to achieve stable and active RuO2 electrocatalyst. Here, the authors report breaking stability and activity limits of RuO2 by constructing a RuO2/CoOx interface.
- Kun Du
- , Lifu Zhang
- & Tao Ling
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Article
| Open AccessTackling realistic Li+ flux for high-energy lithium metal batteries
The low conductivity of LiF disturbs Li+ diffusion across solid electrolyte interphase (SEI) and induces Li+ transfer-driven dendritic growth. Herein, the authors establish a mechanistic model to decipher how the SEI affects realistic Li plating in high-fluorine electrolytes.
- Shuoqing Zhang
- , Ruhong Li
- & Xiulin Fan
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Article
| Open AccessSelf-repairing interphase reconstructed in each cycle for highly reversible aqueous zinc batteries
Metallic zinc is an ideal anode material for aqueous rechargeable batteries but reversibility is a challenge. Here, the authors realise a dynamic real-time reconstructed interphase on zinc anode formed by graphitic carbon nitride quantum dot as an electrolyte additive to improve the performance of Zn metal anodes.
- Wenyao Zhang
- , Muyao Dong
- & Zhi Li
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Comment
| Open AccessThe role of concentration in electrolyte solutions for non-aqueous lithium-based batteries
The quest for high-energy electrochemical energy storage systems has driven researchers to look toward highly concentrated electrolytes. Here, the author discusses the recent progress and future perspectives of such electrolytes and their ability to improve the performances of lithium-based batteries.
- Guinevere A. Giffin
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Article
| Open AccessExtending the low-temperature operation of sodium metal batteries combining linear and cyclic ether-based electrolyte solutions
The low-temperature operation of non-aqueous sodium-based batteries is affected by the properties of the electrolyte. Here the authors propose specific electrolyte formulations that are thermally stable down to −150 °C and enable a stable electrode|electrolyte interface at low temperatures.
- Chuanlong Wang
- , Akila C. Thenuwara
- & Weiyang Li
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Comment
| Open AccessThe defect challenge of wide-bandgap semiconductors for photovoltaics and beyond
The optoelectronic performance of wide-bandgap semiconductors often cannot compete with that of their defect-tolerant small-bandgap counterpart. Here, the authors outline three main challenges to overcome for mitigating the impact of defects in wide-bandgap semiconductors.
- Alex M. Ganose
- , David O. Scanlon
- & Robert L. Z. Hoye
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Article
| Open AccessBoosting the stability of perovskites with exsolved nanoparticles by B-site supplement mechanism
The instability of perovskites with exsolved nanoparticles for CO2 electrocatalysis impedes their practical applications. Here, the authors show the formation of B-site vacancies in perovskite substrate as a major contributor to the degradation and report a strategy to enhance the stability of the perovskites at high voltages.
- Bo-Wen Zhang
- , Meng-Nan Zhu
- & Jing-Li Luo
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Article
| Open AccessInsights into the activity of nickel boride/nickel heterostructures for efficient methanol electrooxidation
Understanding the role of active sites in electrooxidation reactions is important yet challenging. Here, the authors use operando spectroscopies to monitor the effect of methanol concentration on Ni3B/Ni heterostructures during formate production.
- Yanbin Qi
- , Yue Zhang
- & Chunzhong Li
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Article
| Open AccessThe role of solid solutions in iron phosphate-based electrodes for selective electrochemical lithium extraction
Lithium extraction from dilute sources could help solve the lithium supply security issue. Here, the authors investigate the Li- and Na- ion co-intercalation behavior in iron phosphate electrodes and demonstrate the lithium selectivity control through intercalation kinetic manipulations.
- Gangbin Yan
- , George Kim
- & Chong Liu
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Article
| Open AccessNon-fluorinated non-solvating cosolvent enabling superior performance of lithium metal negative electrode battery
Localised high-concentration electrolyte is key to prevent uneven growth of lithium metal by forming a mechanically stable solid-electrolyte interphase. Here, the authors identify the suitable physicochemical properties for non-solvating co-solvents that improve the performance of lithium metal battery.
- Junyeob Moon
- , Dong Ok Kim
- & Jongwoo Lim
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Article
| Open AccessRational design of a topological polymeric solid electrolyte for high-performance all-solid-state alkali metal batteries
Solid-state polymer electrolytes are crucial for developing future rechargeable batteries, but they are still limited in performance. Here, the authors designed a topological polymeric solid electrolyte, enabling an all-solid-state high-voltage lithium metal pouch cell to cycle 200 times efficiently.
- Yun Su
- , Xiaohui Rong
- & Yong-Sheng Hu
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Article
| Open AccessCalcium-tin alloys as anodes for rechargeable non-aqueous calcium-ion batteries at room temperature
The key challenge for rechargeable Ca batteries originates from the severe passivation of the calcium metal anode in electrolyte solutions. Here, the authors demonstrate the feasibility and elucidate the electrochemical properties of calcium-tin (Ca–Sn) alloy anodes for rechargeable Ca batteries.
- Zhirong Zhao-Karger
- , Yanlei Xiu
- & Maximilian Fichtner
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Article
| Open AccessBoosting electrocatalytic CO2–to–ethanol production via asymmetric C–C coupling
It is of high interest to convert CO2 into valuable ethanol product. Here the authors demonstrate the asymmetric C-C coupling triggered on Ag-modified oxide-derived Cu sites can accelerate and steer the reaction pathway for ethanol production with high faradaic efficiency and current density.
- Pengtang Wang
- , Hao Yang
- & Shi-Zhang Qiao
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Article
| Open AccessEffect of the grain arrangements on the thermal stability of polycrystalline nickel-rich lithium-based battery cathodes
Enhancing the stability of positive electrodes at thermally-abused conditions is vital for next-generation lithium-based batteries. Here, the authors report in situ physicochemical characterizations to improve the fundamental understanding of the degradation mechanism in polycrystalline Ni-rich cathodes.
- Dong Hou
- , Zhengrui Xu
- & Feng Lin
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Article
| Open AccessNiobium-doped layered cathode material for high-power and low-temperature sodium-ion batteries
The practical application of sodium-ion batteries at subzero temperatures is hindered by the slow Na-ion transfer kinetics. Here, the authors reported the niobium doping of P2-type cathode active material capable of efficient battery cycling at low temperatures such as −40 °C.
- Qinhao Shi
- , Ruijuan Qi
- & Yufeng Zhao
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Article
| Open AccessExpanding the active charge carriers of polymer electrolytes in lithium-based batteries using an anion-hosting cathode
The energy content of secondary batteries is often limited by the charge carriers available in the system. Here, the authors employed an anion acceptor cathode for simultaneous use of electrolyte anions and cations as effective charge carriers in solid polymer electrolytes for lithium-based batteries.
- Zongjie Sun
- , Kai Xi
- & Shujiang Ding
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Article
| Open AccessDevelopment of efficient aqueous organic redox flow batteries using ion-sieving sulfonated polymer membranes
Aqueous organic redox flow batteries are promising for grid-scale energy storage, although their practical application is still limited. Here, the authors report highly ion-conductive and selective polymer membranes, which boost the battery’s efficiency and stability, offering cost-effective electricity storage.
- Chunchun Ye
- , Anqi Wang
- & Qilei Song
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Article
| Open AccessSmall reorganization energy acceptors enable low energy losses in non-fullerene organic solar cells
Minimising energy loss is important for achieving high-performance organic solar cells. Here, the authors design and synthesise two acceptors with small reorganisation energies and reveal the relationship between reorganisation energy and energy losses.
- Yanan Shi
- , Yilin Chang
- & Zhixiang Wei
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Article
| Open AccessEliminating the need for anodic gas separation in CO2 electroreduction systems via liquid-to-liquid anodic upgrading
In the electrified conversion of CO2 to multicarbon products, CO2 crossover to the O2-rich anodic stream adds a further, energy-intensive, chemical separation step. Here, the authors demonstrate a strategy that eliminates the separation requirement.
- Ke Xie
- , Adnan Ozden
- & Edward H. Sargent
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Article
| Open AccessPhase-transition tailored nanoporous zinc metal electrodes for rechargeable alkaline zinc-nickel oxide hydroxide and zinc-air batteries
Secondary alkaline Zn-based batteries are limited in terms of cycle life. Here, the authors report a nanoporous Zn electrode that stabilizes the electrochemical transition between Zn and ZnO and improves the cycling performance of rechargeable alkaline zinc-based batteries.
- Liangyu Li
- , Yung Chak Anson Tsang
- & Qing Chen
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Article
| Open AccessProduction of a hybrid capacitive storage device via hydrogen gas and carbon electrodes coupling
Conventional electric double-layer capacitors show limited energy content for energy storage applications. Here, the authors report an electrocatalytic hydrogen gas capacitor with improved specific energy, which can operate in pH-universal aqueous electrolyte solutions and a wide temperature range.
- Zhengxin Zhu
- , Zaichun Liu
- & Wei Chen
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Article
| Open AccessRedox-homogeneous, gel electrolyte-embedded high-mass-loading cathodes for high-energy lithium metal batteries
The development of high energy lithium metal batteries is affected by the mass loading of the cathode. Here, the authors report a lithium metal pouch cell with a cathode capacity of 12 mAh cm-2. The positive electrode is prepared by applying UV-curable gel electrolyte as a processing solvent.
- Jung-Hui Kim
- , Ju-Myung Kim
- & Sang-Young Lee
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Article
| Open AccessColossal barocaloric effects with ultralow hysteresis in two-dimensional metal–halide perovskites
Barocaloric materials, undergoing thermal changes in response to applied pressure, may provide energy efficient and zero-emission solid-state cooling. Here the authors report a mechanism for achieving large reversible barocaloric effects near ambient temperature, leveraging volume and conformational entropy changes within the organic bilayers of two-dimensional metal–halide perovskites.
- Jinyoung Seo
- , Ryan D. McGillicuddy
- & Jarad A. Mason
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Article
| Open AccessA cost-effective alkaline polysulfide-air redox flow battery enabled by a dual-membrane cell architecture
Polysulfide-air redox flow batteries are an appealing energy storage technology but suffer from polysulfide crossover and the use of costly catalysts. Here, the authors report a cell structure that enables battery operation using a cost-effective catalyst while mitigating polysulfide crossover.
- Yuhua Xia
- , Mengzheng Ouyang
- & Nigel P. Brandon
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Article
| Open AccessUltrasensitive barocaloric material for room-temperature solid-state refrigeration
A small driving pressure is desirable for practical application of barocaloric materials. Here, the authors demonstrate a sensitive barocaloric effect in NH4I due to strong reorientation-vibration coupling.
- Qingyong Ren
- , Ji Qi
- & Bing Li
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Article
| Open AccessProduction of fast-charge Zn-based aqueous batteries via interfacial adsorption of ion-oligomer complexes
Aqueous zinc batteries attract interest because of their potential for cost-effective and safe electricity storage. Here, the authors develop an in situ formed ion-oligomer nanometric interphase strategy to enable fast-charge aqueous Zn cells.
- Shuo Jin
- , Jiefu Yin
- & Lynden A. Archer
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Article
| Open AccessArgyrodite-type advanced lithium conductors and transport mechanisms beyond paddle-wheel effect
Fundamental mechanisms governing the superionic behaviour in solid-state Li-ion batteries are under debate. Here the authors investigate computationally the mechanism of superionic lithium-ion conduction and predict new advanced lithium superionic conductors.
- Hong Fang
- & Puru Jena
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Article
| Open AccessActive and conductive layer stacked superlattices for highly selective CO2 electroreduction
It is important yet challenging to improve the interface contact between commonly used carbon conductive layer and metal oxide catalysts. Here the authors propose BiCuSeO with alternant active [Bi2O2]2+ sublayers and conductive [Cu2Se2]2- sublayer within its superlattice as efficient catalyst for CO2 electroreduction to formate.
- Junyuan Duan
- , Tianyang Liu
- & Tianyou Zhai
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Article
| Open AccessIn situ dual doping for constructing efficient CO2-to-methanol electrocatalysts
Production of methanol from CO2 electroreduction is attractive but achieving high selectivity, current density and stability simultaneously remains a grand challenge. Here, the authors present an in situ dual doping strategy to construct efficient CO2-to-methanol electrocatalysts.
- Pengsong Li
- , Jiahui Bi
- & Buxing Han
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Article
| Open AccessEnabling fast-charging selenium-based aqueous batteries via conversion reaction with copper ions
Aqueous battery Se-based cathodes are based on a two-electron transfer electrochemical reaction and generally show inadequate rate capability behaviour. Here, the authors propose a four-electron Se chemistry with copper ions as charge carriers to enable fast-charging battery cycling.
- Chunlong Dai
- , Linyu Hu
- & Liangti Qu
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Article
| Open AccessSelective photocatalytic CO2 reduction in aerobic environment by microporous Pd-porphyrin-based polymers coated hollow TiO2
While selective CO2 reduction is crucial for its removal from the environment, the presence of O2 hinders this process. Here authors show CO2 photoreduction in the presence of O2 by incorporating Pd(II) sites into a coordination polymer on TiO2 to selectively adsorb CO2.
- Yajuan Ma
- , Xiaoxuan Yi
- & Jingyu Wang
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Article
| Open AccessA dual-function liquid electrolyte additive for high-energy non-aqueous lithium metal batteries
Lithium metal batteries suffer from poor (electro)chemical stability of the electrodes during prolonged cycling. Here, the authors report a dual function liquid electrolyte additive to form protective interphases on both electrodes to produce lab-scale high energy lithium metal batteries.
- Yuji Zhang
- , Yuan Wu
- & Chengxin Wang
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Article
| Open AccessComplementary Operando Spectroscopy identification of in-situ generated metastable charge-asymmetry Cu2-CuN3 clusters for CO2 reduction to ethanol
Copper-based materials can convert carbon dioxide into multi-carbon products but suffer from poor activity and selectivity. Here, the authors report CuO clusters supported on nitrogen-doped carbon nanosheets for the reduction CO2-to-ethanol, and investigate the change in the catalytic sites while in operation.
- Xiaozhi Su
- , Zhuoli Jiang
- & Yu Wang
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Review Article
| Open AccessSelf-healing oxygen evolution catalysts
Large scale sustainable energy storage by water splitting benefits from performing the oxygen evolution reaction under a variety of conditions. Here, the authors discuss self-healing catalysis as a new tool in the design of stable and functionally active catalysts in acidic to basic solutions, and a variety of water sources
- Agnes E. Thorarinsdottir
- , Samuel S. Veroneau
- & Daniel G. Nocera
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Article
| Open AccessProduction of a monolithic fuel cell stack with high power density
The transportation sector is gradually evolving to become independent of fossil fuels. Here, the authors report a metal-based monolithic solid oxide fuel cell with a power density of 5.6 kW/L suitable for transport applications.
- Stéven Pirou
- , Belma Talic
- & Anke Hagen
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Article
| Open AccessOptical sensors for operando stress monitoring in lithium-based batteries containing solid-state or liquid electrolytes
Chemo-mechanical stress within Li-based batteries detrimentally affects the performance and lifetime of these devices. Here, the authors propose an operando technique using optical fibers embedded in electrodes for internal stress monitoring of cells containing either solid or liquid electrolytes.
- Laura Albero Blanquer
- , Florencia Marchini
- & Jean-Marie Tarascon
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Article
| Open AccessSplicing the active phases of copper/cobalt-based catalysts achieves high-rate tandem electroreduction of nitrate to ammonia
Electrocatalytic recycling of waste nitrate to NH3 under ambient conditions maybe an appealing alternative to the Haber−Bosch process. Here the authors report a tandem catalyst system involving cooperative adsorption of reaction intermediate on different transition metal active sites for nitrate electroreduction with high efficiency.
- Wenhui He
- , Jian Zhang
- & Wolfgang Schuhmann
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Article
| Open AccessA new approach exploiting thermally activated delayed fluorescence molecules to optimize solar thermal energy storage
Direct conversion of solar energy to stored chemical energy can be achieved through photoisomerization. Here, authors exploit thermally activated delayed fluorescence materials as a photosensitizer and signal transducer to harness solar energy, to maximize solar spectrum harvesting without sacrificing energy storage time.
- Fan-Yi Meng
- , I-Han Chen
- & Pi-Tai Chou
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Article
| Open AccessA metal-supported single-atom catalytic site enables carbon dioxide hydrogenation
Converting CO2 and H2O into value-added chemical feedstocks and fuels offers a carbon neutral approach to tackling global energy and climate concerns. Here the authors report a metal supported single-atom catalytic site enabling the electrocatalytic reduction of CO2 to methane.
- Sung-Fu Hung
- , Aoni Xu
- & Edward H. Sargent
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Article
| Open AccessUnraveling the rate-limiting step of two-electron transfer electrochemical reduction of carbon dioxide
Electroreduction of CO2 is heavily investigated but its reaction mechanism needs to be further explored. Here, the authors investigate pH dependency and kinetic isotope effect with respect to the rate expression of CO2 electroreduction to gain further insights into the rate-limiting step.
- Wanyu Deng
- , Peng Zhang
- & Jinlong Gong
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Article
| Open AccessFew-layer bismuth selenide cathode for low-temperature quasi-solid-state aqueous zinc metal batteries
The performances of rechargeable batteries are detrimentally affected by low temperatures (e.g., < 0 °C). Here, the authors report a few-layer Bi2Se3 material capable of improving battery cycling performances when operational temperatures are shifted from +25 °C to −20 °C.
- Yuwei Zhao
- , Yue Lu
- & Chunyi Zhi
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Article
| Open AccessManipulating the oxygen reduction reaction pathway on Pt-coordinated motifs
Controlling O2 reduction pathways can help optimize catalytic activity and product selectivity. Here the authors report facile manipulation of 2e‒ /4e‒ pathways on Pt-coordinated motifs by varying the Pt site density or the coordination environment.
- Jiajun Zhao
- , Cehuang Fu
- & Kun Jiang
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Article
| Open AccessOperando monitoring of ion activities in aqueous batteries with plasmonic fiber-optic sensors
Operando tracking the ion dynamics/states of battery is critical to understanding of electrolyte-electrode interactions. Here the authors propose to use the surface plasmon waves to rapidly screen localized electrochemical events on a sub-μm-scale thickness adjacent to the electrode interface, without perturbing battery operation.
- Runlin Wang
- , Haozhe Zhang
- & Tuan Guo
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Article
| Open AccessAu-activated N motifs in non-coherent cupric porphyrin metal organic frameworks for promoting and stabilizing ethylene production
Metal-organic frameworks are promising catalysts for CO2 electroreduction, yet limited by their poor conductivity and stability. Here, Au nanoneedles are inserted into the metalloporphyrin framework to activate C-C coupling and stabilize the structure for much enhanced ethylene production.
- Xulan Xie
- , Xiang Zhang
- & Yang Peng
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Article
| Open AccessSingle-dispersed polyoxometalate clusters embedded on multilayer graphene as a bifunctional electrocatalyst for efficient Li-S batteries
Efficient electrochemical energy storage in Li-S batteries is hindered by sluggish sulfur redox reactions. Here, the authors propose a polyoxometalate/multilayer graphene composite as a bifunctional electrocatalyst for battery performance improvement.
- Jie Lei
- , Xiao-Xiang Fan
- & Jia-Jia Chen
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Article
| Open AccessCharge-transfer regulated visible light driven photocatalytic H2 production and CO2 reduction in tetrathiafulvalene based coordination polymer gel
Designing active materials for efficient photocatalysis are of great interests. Herein the authors report coordination polymer gel assembled by low molecular weight gelator as photocatalysts for visible light driven H2 production and CO2 reduction regulated by charge-transfer interactions.
- Parul Verma
- , Ashish Singh
- & Tapas Kumar Maji
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Article
| Open AccessImproving the alkali metal electrode/inorganic solid electrolyte contact via room-temperature ultrasound solid welding
The practical application of solid-state rechargeable alkali metal batteries is hindered by the poor contact between the metal electrode and the solid electrolyte. Here, the authors report an ultrasound solid welding strategy to favor the contact between these cells components.
- Xinxin Wang
- , Jingjing Chen
- & Zhiyong Mao