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| Open AccessDynamical evolution of CO2 and H2O on garnet electrolyte elucidated by ambient pressure X-ray spectroscopies
Li6.5La3Zr1.5Ta0.5O12 (LLZO) is a promising solid electrolyte but suffers from severe surface degradation in air. Here, authors use mapping of resonant Auger spectroscopy and various ambient pressure X-ray spectroscopies to elucidate the dynamical evolution of CO2 and H2O on clean LLZO surfaces.
- Nian Zhang
- , Guoxi Ren
- & Xiaosong Liu
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Article
| Open AccessUltrastable halide perovskite CsPbBr3 photoanodes achieved with electrocatalytic glassy-carbon and boron-doped diamond sheets
Perovskites are desirable for photoelectrochemical applications but are unstable in aqueous electrolytes. Here, the authors report a perovskite photoanode in aqueous electrolyte, preserving 95% photocurrent density after over 100 h of operation.
- Zhonghui Zhu
- , Matyas Daboczi
- & Salvador Eslava
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Article
| Open AccessConstructing regulable supports via non-stoichiometric engineering to stabilize ruthenium nanoparticles for enhanced pH-universal water splitting
Establishing optimal metal-support interactions is crucial for creating efficient catalysts for water splitting. Here, stable Ti–O–Ru interface formation and minimal work function difference between Ru nanoparticles and non-stoichiometric Ti4O7 lead to exceptional bifunctional activity of Ru/Ti4O7 for both HER and OER across pH-universal environments, maintaining stable operation for 500 h.
- Sheng Zhao
- , Sung-Fu Hung
- & Shengjie Peng
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Article
| Open AccessHarnessing strong aromatic conjugation in low-dimensional perovskite heterojunctions for high-performance photovoltaic devices
The large organic cations in low-dimensional perovskite often introduces carrier mobility anisotropy and impedes charge transport. Here, authors report perovskite heterojunction with strong aromatic conjugated perovskites, realizing certified efficiency of over 25% in stable perovskite solar cells.
- Bo Li
- , Qi Liu
- & Zonglong Zhu
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Article
| Open AccessAn integrated high-throughput robotic platform and active learning approach for accelerated discovery of optimal electrolyte formulations
Solubility determines energy density in redox flow batteries. Here, authors combine automated experiments with machine learning to efficiently identify solvents that significantly enhance solubility, testing less than 10% of over 2000 candidates.
- Juran Noh
- , Hieu A. Doan
- & Yangang Liang
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Article
| Open AccessSynergistically optimized electron and phonon transport in high-performance copper sulfides thermoelectric materials via one-pot modulation
It is hard to simultaneously improve electrical and thermal properties of materials due to the strong coupling of carrier and phonon transport. Here, the authors propose a one-pot modulation strategy for simultaneously adjusting carrier and phonon transport in copper sulfids.
- Yi-Xin Zhang
- , Qin-Yuan Huang
- & Zhen-Hua Ge
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Article
| Open AccessSingle [0001]-oriented zinc metal anode enables sustainable zinc batteries
The authors present a single [0001]-oriented Zn metal anode with high reversibility and demonstrate the significance of the Zn(0002) metal anode, characterized by a single crystalline orientation, for promoting ultra-sustainable homoepitaxial growth.
- Xiaotan Zhang
- , Jiangxu Li
- & Jiang Zhou
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Article
| Open AccessUnderstanding the effect of spatially separated Cu and acid sites in zeolite catalysts on oxidation of methane
Methane is a potent greenhouse gas, and its removal is critical. Here, the authors demonstrate that spatially separated Cu and acid sites in Cu/zeolites influence product distribution and efficiency for methane oxidation.
- Peipei Xiao
- , Yong Wang
- & Toshiyuki Yokoi
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Article
| Open AccessCreation of flexible spin-caloritronic material with giant transverse thermoelectric conversion by nanostructure engineering
Nanostructure engineering enables transforming simple magnetic alloys into spincaloritronic materials with large transverse thermoelectric conversion. This has led to a high anomalous Nernst coefficient in flexible Fe-based amorphous alloys.
- Ravi Gautam
- , Takamasa Hirai
- & Hossein Sepehri-Amin
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Article
| Open AccessDecreasing exciton dissociation rates for reduced voltage losses in organic solar cells
The device’s electroluminescence efficiency is vital to reduce non-radiative voltage losses and boost organic solar cell performance. Here, the authors demonstrate that this efficiency is influenced not only by the decay of charge transfer states but also by the dissociation of singlet states.
- Hongbo Wu
- , Hao Lu
- & Zheng Tang
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Article
| Open AccessKeto-anthraquinone covalent organic framework for H2O2 photosynthesis with oxygen and alkaline water
Hydrogen peroxide photosynthesis is an important reaction that suffers from poor activity due to the high energy barrier of hydrogen extraction in water. Here, we report a keto-form anthraquinone framework that shows promising performance in alkaline conditions.
- Xiangcheng Zhang
- , Silian Cheng
- & Lizhi Zhang
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Article
| Open AccessSolar-driven sugar production directly from CO2 via a customizable electrocatalytic–biocatalytic flow system
Solar-driven artificial food synthesis from CO2 provides an approach to overcome the limitations of natural photosynthesis, but it is very challenging. Here, the authors report a hybrid electrocatalytic-biocatalytic flow system, coupling photovoltaics-powered electrocatalysis (CO2 to formate) with a five enzyme cascade platform (formate to sugar), which achieves conversion of CO2 to C6 sugar (L-sorbose) with a solar-to-food energy conversion efficiency of 3.5%.
- Guangyu Liu
- , Yuan Zhong
- & Yujie Xiong
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Article
| Open AccessInduced dipole moments in amorphous ZnCdS catalysts facilitate photocatalytic H2 evolution
The rapid recombination of photogenerated charge carriers is a key challenge for photocatalytic hydrogen production. Here, the authors report an amorphous ZnCdS to break the symmetry of atom arrangement that induces strong dipole fields, thus providing extra driving forces for charge separation.
- Xin Wang
- , Boyan Liu
- & Songcan Wang
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Article
| Open AccessVacancies tailoring lattice anharmonicity of Zintl-type thermoelectrics
Vacancies are traditionally considered to play a role of phonon-defect scattering. Here, the authors show that vacancies can induce phonon softening, enhance phonon anharmonicity, and cause a dramatic reduction in the lattice thermal conductivity.
- Jinfeng Zhu
- , Qingyong Ren
- & Jie Ma
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Article
| Open AccessSpectroscopic visualization of reversible hydrogen spillover between palladium and metal–organic frameworks toward catalytic semihydrogenation
The authors report an in situ investigation of interfacial hydrogen spillover in Pd/ZIF-8 structures with X-ray and Raman techniques. A mechanistic picture of how Pd/ZIF-8 catalyst mediate alkyne semihydrogenation to alkynes is described.
- Qiaoxi Liu
- , Wenjie Xu
- & Yujie Xiong
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Article
| Open AccessStrain regulates the photovoltaic performance of thick-film perovskites
The power conversion efficiencies of thick-film perovskite solar cells lag behind those with nanometre film thickness. Here, the authors rule out the restrictions of carrier lifetime on device performance and reveal the critical role of lattice strain in micron-scale thick perovskite films.
- Pengju Shi
- , Jiazhe Xu
- & Rui Wang
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Article
| Open AccessAn entanglement association polymer electrolyte for Li-metal batteries
Here, the authors report an entanglement association polymer electrolyte with a polymer matrix and copolymer stabilizer. The developed entangled structure forms a stable interface for the polymer electrolyte during charging and discharging.
- Hangchao Wang
- , Yali Yang
- & Dingguo Xia
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Article
| Open AccessExtreme Li-Mg selectivity via precise ion size differentiation of polyamide membrane
Achieving high selectivity of Li+ and Mg2+ is of paramount importance for effective lithium extraction from brines, and nanofiltration (NF) membrane plays a critical role in this process. Here the authors report the fabrication of polyamide NF membranes with ultra-high Li + /Mg2+ selectivity by modifying the interfacial polymerization process with an oil-soluble surfactant.
- Quan Peng
- , Ruoyu Wang
- & Lei Jiang
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Article
| Open AccessA restricted dynamic surface self-reconstruction toward high-performance of direct seawater oxidation
Chlorine evolution reaction and deep reconstruction of catalyst are critical issues in direct seawater electrolysis. Here, the authors propose a MoO3/CoO/carbon composite material for improved selective seawater oxidation and restricted dynamic surface self-reconstruction.
- Ling Zhou
- , Daying Guo
- & Shun Wang
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Article
| Open AccessPulse potential mediated selectivity for the electrocatalytic oxidation of glycerol to glyceric acid
Mitigating the deactivation of noble metal-based catalysts caused by self-oxidation and toxic adsorption poses a considerable challenge in organic electro-oxidation. This study addresses the issue by employing a pulsed potential electrolysis approach to selectively electrocatalyze the oxidation of glycerol to glyceric acid using a Pt-based catalyst.
- Wei Chen
- , Liang Zhang
- & Yuqin Zou
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Article
| Open AccessPhenol as proton shuttle and buffer for lithium-mediated ammonia electrosynthesis
The proton shuttle plays a critical role in the proton transfer process during lithium-mediated ammonia synthesis. Here, the authors establish the structure-activity relationship and design principles for effective proton shuttles.
- Xianbiao Fu
- , Aoni Xu
- & Ib Chorkendorff
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Article
| Open AccessWell-defined diatomic catalysis for photosynthesis of C2H4 from CO2
Principal interest lies in diatomic catalysts (DACs) for efficient CO2 to C2H4 photoconversion yet optimizing catalytic performance and exploring reaction mechanisms are impeded by heteronuclear atom random distribution. Here, a novel up-bottom ion-cutting architecture is proposed for fabricating well-defined DACs.
- Zhongkai Xie
- , Shengjie Xu
- & Shuyan Song
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Article
| Open AccessAssessing intra- and inter-molecular charge transfer excitations in non-fullerene acceptors using electroabsorption spectroscopy
The performance of Y6-containing donor-acceptor active layers in organic solar cells is highly related to the charge-transfer nature in Y6 aggregates. Here, authors study charge-transfer characteristics of excitations of isolated and aggregated Y6 molecules through electroabsorption spectroscopy.
- Sudhi Mahadevan
- , Taili Liu
- & Sai-Wing Tsang
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Article
| Open AccessHigh figure-of-merit for ZnO nanostructures by interfacing lowly-oxidized graphene quantum dots
It is crucial to design ZnO with uniform nanoscale features to reduce thermal conductivity while maintaining electrical conduction pathways. Authors realize a high figure-of-merit value of 0.486 at 580 K by interfacing graphene quantum dots with three-dimensional nanostructured ZnO.
- Myungwoo Choi
- , Juyoung An
- & Seokwoo Jeon
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Article
| Open AccessCapturing ion trapping and detrapping dynamics in electrochromic thin films
Ion trapping has been found to be responsible for the performance degradation in electrochromic oxide thin films. This paper visualizes ion trapping and detrapping dynamics, and provides a general picture of electrochromism in amorphous WO3.
- Renfu Zhang
- , Qinqi Zhou
- & Rui-Tao Wen
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Article
| Open AccessIntragrain impurity annihilation for highly efficient and stable perovskite solar cells
The detrimental effects of intragrain impurity nanoclusters on the efficiency and stability of perovskite solar cells remain unexplored. Here, the authors study the intragrain impurity annihilation by in situ scanning transmission electron microscopy and adopt a laser stimulus to heal such impurity.
- Songhua Cai
- , Zhipeng Li
- & Yuanyuan Zhou
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Article
| Open AccessDirect observation of tunable thermal conductance at solid/porous crystalline solid interfaces induced by water adsorbates
Interfacial thermal transfer is critical for heat dissipation of devices with interfaces. Here, the authors propose a strategy to tune the interfacial thermal transport between substrate and metal-organic frameworks to benefit their related cooling applications.
- Guang Wang
- , Hongzhao Fan
- & Yanguang Zhou
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Article
| Open AccessMixed tin-lead perovskites with balanced crystallization and oxidation barrier for all-perovskite tandem solar cells
The disparity in crystallization processes between tin- and lead-based perovskites has been a dominant factor contributing to high defect densities. Here, authors employ a functional molecule to inhibit tin oxidation, realizing monolithic all-perovskite tandems with certified efficiency over 27%.
- Jin Zhou
- , Shiqiang Fu
- & Weijun Ke
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Article
| Open AccessSupra-biological performance of immobilized enzymes enabled by chaperone-like specific non-covalent interactions
Designing complex synthetic materials for enzyme immobilization could unlock the utility of biocatalysis in extreme environments. Here, the authors report on random copolymer brushes as dynamic immobilization supports that enable supra-biological catalytic performance of immobilized enzymes.
- Héctor Sánchez-Morán
- , Joel L. Kaar
- & Daniel K. Schwartz
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Article
| Open AccessA solid-state lithium-ion battery with micron-sized silicon anode operating free from external pressure
Applying high stack pressure is primarily done to address the mechanical failure issue of solid-state batteries. Here, the authors propose a mechanical optimization strategy involving elastic electrolyte to realize solid-state batteries operating without external pressurizing.
- Hui Pan
- , Lei Wang
- & Haoshen Zhou
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Article
| Open AccessSingle-atom Mo-tailored high-entropy-alloy ultrathin nanosheets with intrinsic tensile strain enhance electrocatalysis
Atomically precise modification of high-entropy alloys is highly appealing for electrocatalysis. Here, the authors design single-atom Mo-tailored high-entropy alloy nanosheets with dilute Pt-Pt ensembles and intrinsic tensile strain for promoting methanol electro-oxidation towards formate.
- Lin He
- , Menggang Li
- & Shaojun Guo
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Article
| Open AccessLiquid metals for boosting stability of zeolite catalysts in the conversion of methanol to hydrocarbons
For the methanol-to-hydrocarbons process, coke build can rapidly deactivate the zeolite catalyst. Here the authors show that the addition of liquid metal gallium can reduce coke deposition and increase catalyst lifetime.
- Yong Zhou
- , Sara Santos
- & Vitaly V. Ordomsky
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Article
| Open AccessTuning polymer-backbone coplanarity and conformational order to achieve high-performance printed all-polymer solar cells
All-polymer solar cells comprising both polymeric donors and acceptors offer better morphological and mechanical stability, and a broader processing window for printing. Here, the authors report a polymer acceptor based on bithiazole linker with more coplanar and ordered molecular conformation.
- Yilei Wu
- , Yue Yuan
- & Zhenan Bao
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Article
| Open AccessDeciphering the contributing motifs of reconstructed cobalt (II) sulfides catalysts in Li-CO2 batteries
Improving catalyst efficiency is vital for Li-CO2 batteries, but understanding catalyst structures during battery operation is hard. Here, the authors uncover catalyst reconstruction and its link to activity, highlighting a self-constructed oxysulfide structure with high activity and stability in Li-CO2 batteries.
- Yingqi Liu
- , Zhiyuan Zhang
- & Hui-Ming Cheng
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Article
| Open AccessA Ce-CuZn catalyst with abundant Cu/Zn-OV-Ce active sites for CO2 hydrogenation to methanol
Carbon dioxide hydrogenation is an important industrial reaction. Here, the authors design a CeCuZn catalyst through a metal organic framework template for CO2 hydrogenation to methanol with excellent methanol yield and stability.
- Runping Ye
- , Lixuan Ma
- & Jian Liu
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Article
| Open AccessProton-selective coating enables fast-kinetics high-mass-loading cathodes for sustainable zinc batteries
Sluggish Zn2+-dominated Faradic reactions lead to suboptimal charge-storage capacity and durability of aqueous zinc battery cathodes. Here, the authors present a proton-selective interfacial coating strategy that enables high-performance cathodes with fast-kinetics proton-dominated Faradic reactions.
- Quanquan Guo
- , Wei Li
- & Xinliang Feng
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Article
| Open AccessInter-site structural heterogeneity induction of single atom Fe catalysts for robust oxygen reduction
Here, authors report an inter-site structural heterogeneity induced effect of hierarchical single atom Fe catalysts for robust oxygen reduction. Dynamic evolutions and insights into structure-activity relationship are presented.
- Peng Zhang
- , Hsiao-Chien Chen
- & Yuan Pan
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Article
| Open AccessSupramolecular catalyst with [FeCl4] unit boosting photoelectrochemical seawater splitting via water nucleophilic attack pathway
The strongly coupled interface between molecular catalysts and light absorbers is the key to solving efficient photoelectrochemical water oxidation. An in situ polymerized supramolecular-like catalyst was used to couple with BiVO4 for efficient and stable photoelectrochemical seawater splitting
- Jiaming Miao
- , Cheng Lin
- & Kan Zhang
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Article
| Open AccessMolecular anchoring of free solvents for high-voltage and high-safety lithium metal batteries
Advanced electrolyte is essential for high-energy-density lithium metal batteries. Here, the authors design a molecular anchoring dilute electrolyte via intermolecular hydrogen bonding with free solvents to improve the battery electrochemical and thermal stabilities.
- Zhuangzhuang Cui
- , Zhuangzhuang Jia
- & Xiaodi Ren
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Article
| Open AccessThe dynamic adsorption affinity of ligands is a surrogate for the passivation of surface defects
Semiconductor defects persist as a source of energy loss in solar cells. Here, the authors use ab initio simulations to reveal overlooked defect dynamics, guiding passivator design for enhanced photovoltaic performance.
- Jian Xu
- , Aidan Maxwell
- & Edward H. Sargent
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Article
| Open AccessPolymer-acid-metal quasi-ohmic contact for stable perovskite solar cells beyond a 20,000-hour extrapolated lifetime
The development of robust quasi-ohmic contact with minimal resistance, exceptional stability and cost-effectiveness is crucial for practical application of perovskite solar cells. Here, authors report a polymer-acid-metal structure as the contact and realize long photo-thermal-operational stability.
- Junsheng Luo
- , Bowen Liu
- & Yicheng Zhao
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Article
| Open AccessDynamic chloride ion adsorption on single iridium atom boosts seawater oxidation catalysis
The seawater oxidation reaction faces challenges from competitive chloride oxidation reaction. Herein, the authors have utilized chlorine adsorption to modulate the single-atom Ir coordination state and promote seawater oxidation and catalyst stability.
- Xinxuan Duan
- , Qihao Sha
- & Xiaoming Sun
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Article
| Open AccessEfficient all-small-molecule organic solar cells processed with non-halogen solvent
The development of non-halogen solvent processed all-small-molecule organic solar cells was challenging. Here, the authors employ a small molecule donor with strong aggregation property to improve molecular pre-aggregation in tetrahydrofuran, realizing ternary device with efficiency of 16.1%.
- Wei Gao
- , Ruijie Ma
- & Gang Li
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Article
| Open AccessAn acetate electrolyte for enhanced pseudocapacitve capacity in aqueous ammonium ion batteries
Ammonium ion batteries are of growing interest for energy storage research. Here, the authors observe two-step pseudocapacitive storage behavior in an ammonium acetate electrolyte, resulting in a superior ammonium ion storage capacity.
- Zhuoheng Bao
- , Chengjie Lu
- & ZhengMing Sun
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Article
| Open AccessModelling atomic and nanoscale structure in the silicon–oxygen system through active machine learning
Understanding the silicon-oxygen system is crucial for various applications. Here, the authors present an interatomic potential covering a wide range of the Si-O configurational space and showcase applications to silica and Si-SiO2 interfaces.
- Linus C. Erhard
- , Jochen Rohrer
- & Volker L. Deringer
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Article
| Open AccessCation desolvation-induced capacitance enhancement in reduced graphene oxide (rGO)
Understanding local electrochemical processes can help improve electrochemical energy storage. Here, the authors report a charge storage mechanism in aqueous electrolyte for reduced graphene oxide using an electrochemical quartz crystal microbalance.
- Kangkang Ge
- , Hui Shao
- & Patrice Simon
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Article
| Open AccessCharging modulation of the pyridine nitrogen of covalent organic frameworks for promoting oxygen reduction reaction
The catalytic efficacy of covalent organic frameworks (COFs) is constrained by their restricted electro-transfer capability and weak binding affinities for reaction intermediates. Here the authors report COFs with various pyridinic-based units for tuning their catalytic activity towards oxygen reduction reaction.
- Xiubei Yang
- , Qizheng An
- & Gaofeng Zeng
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Article
| Open AccessRational molecular and device design enables organic solar cells approaching 20% efficiency
A systematic design of light-absorbing molecules is challenging for them to satisfy multiple key requirements for efficient solar cell application. Here, the authors optimize halogen substitution position in terminal groups of acceptors for realizing ternary cells with efficiency approaching 20%.
- Jiehao Fu
- , Qianguang Yang
- & Gang Li
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Article
| Open AccessSingle-atom tailored atomically-precise nanoclusters for enhanced electrochemical reduction of CO2-to-CO activity
Tailoring catalytic performance of atomically-precise metal nanoclusters catalysts is of great interest but remains challenging. Here, the authors report a co-eletropolymerization strategy to modify well-defined Au8 nanoclusters by single-atom sites to enhance its electrocatalytic activity for the reduction of CO2 towards CO.
- Yi-Man Wang
- , Fang-Qin Yan
- & Shuang-Quan Zang