Bimetallic In_(2)O_(3)/Bi_(2)O_(3) Catalysts Enable Highly Selective CO_(2) Electroreduction to Formate within Ultra-Broad Potential Windows

CO_(2)electrochemical reduction reaction(CO_(2)RR)to formate is a hopeful pathway for reducing CO_(2)and producing high-value chemicals,which needs highly selective catalysts with ultra-broad potential windows to meet the industrial demands.Herein,the nanorod-like bimetallic ln_(2)O_(3)/Bi_(2)O_(3)catalysts were successfully synthesized by pyrolysis of bimetallic InBi-MOF precursors.The abundant oxygen vacancies generated from the lattice mismatch of Bi_(2)O_(3)and ln_(2)O_(3)reduced the activation energy of CO_(2)to*CO_(2)·^(-)and improved the selectivity of*CO_(2)·^(-)to formate simultaneously.Meanwhile,the carbon skeleton derived from the pyrolysis of organic framework of InBi-MOF provided a conductive network to accelerate the electrons transmission.The catalyst exhibited an ultra-broad applied potential window of 1200 mV(from-0.4 to-1.6 V vs RHE),relativistic high Faradaic efficiency of formate(99.92%)and satisfactory stability after 30 h.The in situ FT-IR experiment and DFT calculation verified that the abundant oxygen vacancies on the surface of catalysts can easily absorb CO_(2)molecules,and oxygen vacancy path is dominant pathway.This work provides a convenient method to construct high-performance bimetallic catalysts for the industrial application of CO_(2)RR.

Strong Interaction Between Redox Mediators and Defect-Rich Carbons Enabling Simultaneously Boosted Voltage Windows and Capacitance for Aqueous Supercapacitors

Energy density,the Achilles’heel of aqueous supercapacitors,is simultaneously determined by the voltage window and specific capacitance of the carbon materials,but the strategy of synchronously boosting them has rarely been reported.Herein,we demonstrate that the rational utilization of the interaction between redox mediators(RMs)and carbon electrode materials,especially those with rich intrinsic defects,contributes to extended potential windows and more stored charges concurrently.Using 4-hydroxy-2,2,6,6-tetramethylpiperidinyloxyl(4OH-TEMPO)and intrinsic defect-rich carbons as the RMs and electrode materials,respectively,the potential window and capacitance are increased by 67%and sixfold in a neutral electrolyte.Moreover,this strategy could also be applied to alkaline and acid electrolytes.The first-principle calculation and experimental results demonstrate that the strong interaction between 4OH-TEMPO and defectrich carbons plays a key role as preferential adsorbed RMs may largely prohibit the contact of free water molecules with the electrode materials to terminate the water splitting at elevated potentials.For the RMs offering weaker interaction with the electrode materials,the water splitting still proceeds with a thus sole increase of the stored charges.The results discovered in this work could provide an alternative solution to address the low energy density of aqueous supercapacitors.

Efficient CO_(2) electroreduction over N-doped hieratically porous carbon derived from petroleum pitch

Developing of economic and efficient catalysts is critical for the application of electroreduction of carbon dioxide to highly valuable chemicals.Herein,we present a facile method to synthesize N-doped hieratically porous carbon through pyrolysis of petroleum pitch followed by ammonia etching.We found mesopores are favored formation by removing of asphaltene from petroleum pitch during the carbonation process.Simultaneously,ammonia etching can not only increase the pyridinic-N content,but also upgrade the ratio of meso-to micro-pores of carbon materials.Using the N-doped hieratically porous carbon as catalyst for carbon dioxide electroreduction,the Faradaic efficiency of carbon monoxide reaches 83%at-0.9 V vs.the reversible hydrogen electrode(RHE)in 0.1 M KHCO_(3).This superior performance is attributed to the synergistic effects of highly pyridinic-N content in conjunction with the hieratically porous architecture,rendering abundant exposed and accessible active sites for electroreduction of CO_(2).Our work provides a new strategy for the large-scale preparation of high-performance,low-cost catalysts for CO_(2) electroreduction.

Propelling polysulfide redox by Fe_(3)C-FeN heterostructure@nitrogendoped carbon framework towards high-efficiency Li-S batteries

Lithium-sulfur(Li-S) batteries hold great promise in next-generation high-energy-density energy storage systems,but the intractable shuttle effect and the sluggish redox kinetics of polysulfides hinder the practical implementation of Li-S batteries.Here,heterostructured Fe_(3)C-FeN nanoparticles dotted in the threedimensional-ordered nitrogen-doped carbon framework(Fe_(3)C-FeN@NCF) were synthesized by molecular engineering combined with heterointerface engineering,and were applied to regulate the immobilization-diffusion-conversion behavior of polar polysulfides.It is experimentally and theoretically demonstrated that the heterointerface between Fe_(3)C and FeN exhibits high sulfiphilicity and high electronic/ionic conductivity,thus effectively capturing polysulfides and accelerating the bidirectional conversion of sulfur species.Meanwhile,the holey carbon framework functions as the scaffold to highly disperse binary nanoparticles,ensuring the sufficient exposure of active sites and the easy accessibility for lithium ions and electrons.By virtue of these synergistic merits,the Li-S batteries based on Fe_(3)CFeN@NCF-modified separators afford excellent electrochemical performances including a high rate capacity of 858 mA h g^(-1)at 2 C and a low capacity decay rate of 0.07% per cycle after 800 cycles at 1C This work provides inspiration for the design of heterostructured compounds and sheds light on the potential of heterostructure in high-efficiency Li-S batteries.

Engineered nitrogen doping on VO_(2)(B)enables fast and reversible zinc-ion storage capability for aqueous zinc-ion batteries

Vanadium-based compounds with high theoretical capacities and relatively stable crystal structures are potential cathodes for aqueous zinc-ion batteries(AZIBs).Nevertheless,their low electronic conductivity and sluggish zinc-ion diffusion kinetics in the crystal lattice are greatly obstructing their practical application.Herein,a general and simple nitrogen doping strategy is proposed to construct nitrogen-doped VO_(2)(B)nanobelts(denoted as VO_(2)-N)by the ammonia heat treatment.Compared with pure VO_(2)(B),VO_(2)-N shows an expanded lattice,reduced grain size,and disordered structure,which facilitates ion transport,provides additional ion storage sites,and improves structural durability,thus presenting much-enhanced zinc-ion storage performance.Density functional theory calculations demonstrate that nitrogen doping in VO_(2)(B)improves its electronic properties and reduces the zinc-ion diffusion barrier.The optimal VO_(2)-N400 electrode exhibits a high specific capacity of 373.7 mA h g^(-1)after 100 cycles at 0.1 A g^(-1)and stable cycling performance after 2000 cycles at 5 A g^(-1).The zinc-ion storage mechanism of VO_(2)-N is identified as a typical intercalation/de-intercalation process.

Intrinsic Mechanisms of Morphological Engineering and Carbon Doping for Improved Photocatalysis of 2D/2D Carbon Nitride Van Der Waals Heterojunction

Van der Waals(VDW)heterojunctions in a 2D/2D contact provide the highest area for the separation and transfer of charge carriers.In this work,a top-down strategy with a gas erosion process was employed to fabricate a 2D/2D carbon nitride VDW heterojunction in carbon nitride(g-C_(3)N_(4))with carbon-rich carbon nitride.The created 2D semiconducting channel in the VDW structure exhibits enhanced electric field exposure and radiation absorption,which facilitates the separation of the charge carriers and their mobility.Consequently,compared with bulk g-C_(3)N_(4)and its nanosheets,the photocatalytic performance of the fabricated carbon nitride VDW heterojunction in the water splitting reaction to hydrogen is improved by 8.6 and 3.3 times,respectively,while maintaining satisfactory photo-stability.Mechanistically,the finite element method(FEM)was employed to evaluate and clarify the contributions of the formation of VDW heterojunction to enhanced photocatalysis,in agreement quantitatively with experimental ones.This study provides a new and effective strategy for the modification and more insights to performance improvement on polymeric semiconductors in photocatalysis and energy conversion.

The Nature of Active Sites for Plasmon-Mediated Photothermal Catalysis and Heat-Coupled Photocatalysis in Dry Reforming of Methane

Solar energy-induced catalysis has been attracting intensive interests and its quantum efficiencies in plasmon-mediated photothermal catalysis(P-photothermal catalysis)and external heat-coupled photocatalysis(E-photothermal catalysis)are ultimately determined by the catalyst structure for photo-induced energetic hot carriers.Herein,different catalysts of supported(TiO_(2)-P25 and Al_(2)O_(3))platinum quantum dots are employed in photo,thermal,and photothermal catalytic dry reforming of methane.Integrated experimental and computational results unveil different active sites(hot zones)on the two catalysts for photo,thermal,and photothermal catalysis.The hot zones of P-photothermal catalysis are identified to be the metal-support interface on Pt/P25 and the Pt surface on Pt/Al_(2)O_(3),respectively.However,a change of the active site to the Pt surface on Pt/P25 is for the first time observed in E-photothermal catalysis(external heating temperature of 700℃).The hot zones contribute to the significant enhancements in photothermal catalytic reactivity against thermocatalysis.This study helps to understand the reaction mechanism of photothermal catalysis to exploit efficient catalysts for solar energy utilization and fossil fuels upgrading.

Selective photocatalytic oxidation of methane to C1 oxygenates by regulating sizes and facets over Au/ZnO

Photocatalytic oxidation of methane to value-added chemicals is a promising process under mild conditions,nevertheless confronting great challenges in efficiently activating C-H bonds and inhibiting over-oxidation.Herein,we propose a comprehensive strategy for the selective generation of reactive oxygen species(ROS)by regulating the sizes and facets of Au nanoparticles loaded on ZnO.For photocatalytic methane oxidation at ambient temperature,a high oxygenates yield of 36.4 mmol·g^(-1)·h^(-1) with a nearly 100%selectivity has been achieved over the optimized 1.0%Au/ZnO-9.6(1%Au with(111)facet and 9.6 nm size on ZnO)photocatalyst,exceeding most reported literatures.Mechanism investigations reveal that 1.0%Au/ZnO-9.6 with the medium size and Au(111)facet guarantees the favourable formation of superoxide radicals(·OOH)through mild oxygen reduction,ultimately leading to excellent photocatalytic methane oxidation performance.This work provides some guidance for the delicate design of photocatalysts for efficient photocatalytic methane oxidation and oxygen utilization.

Revisiting N,S co-doped carbon materials with boosted electrochemical performance in sodium-ion capacitors:The manipulation of internal electric field

Heteroatom doping has emerged as a prevailing strategy to enhance the storage of sodium ions in carbon materials.However,the underlying mechanism governing the performance enhancement remains undisclosed.Herein,we fabricated N/S co-doped carbon beaded fibers(S-N-CBFs),which exhibited glorious rate performance and durableness in Na+storage,showcasing no obvious capacity decay even after 3500 cycles.Furthermore,when used as anodes in sodium-ion capacitors,the S-N-CBFs delivered exceptional results,boasting a high energy density of 225 Wh·kg^(-1),superior power output of 22500 W·kg^(-1),and outstanding cycling stability with a capacity attenuation of merely 0.014%per cycle after 4000 cycles at 2 A·g^(-1).Mechanistic investigations revealed that the incorporation of both pyridinic N and pyrrolic N into the carbon matrix of S-N-CBFs induced internal electric fields(IEFs),with the former IEF being stronger than the latter,in conjunction with the doped S atom.Density functional theory calculations further unveiled that the intensity of the IEF directly influenced the adsorption of Na+,thereby resulting in the exceptional performances of S-N-CBFs as sodium-ion storage materials.This work uncovers the pivotal role of IEF in regulating the electronic structure of carbon materials and enhancing their Na^(+)storage capabilities,providing valuable insights for the development of more advanced electrode materials.

LiOH-mediated crystallization regulating strategy enhancing electrochemical performance and structural stability of SiO anodes for lithium-ion batteries

Silicon monoxide(SiO)is widely recognized as a promising anode material for next-generation lithium-ion batteries.Owing to its metastable amorphous structure,SiO exhibits a highly complex degree of crystallization at the microscopic level,which significantly influences its electrochemical behavior.As a consequence,accurately regulating the crystallization of SiO,and further establishing the relationship between crystallinity and electrochemical performance are very critical for SiO anodes.In this article,carbon-coated SiO materials with different crystallinity degrees were synthesized using lithium hydroxide monohydrate(LiOH·H_(2)O)as a structural modifier to reveal this rule.Additionally,moderate amount of LiOH·H_(2)O addition results in the forming of an oxygen-rich shell,which effectively inhibits the inward migration of oxygen atoms on the SiO surface and suppresses volume expansion.However,the crystallinity of SiO will gradually enhance and the crystalline phase appears with increasing the amount of LiOH·H_(2)O,which will generate a deteriorative Li+diffusion kinetic.After balancing the above two contradictions,a mass fraction of 1%LiOH·H_(2)O for the additive yielded SiO@C-1,characterized by optimal crystallinity.SiO@C-1 demonstrates exceptional long-cycle stability with 74.8%capacity retention after 500 cycles at 1 A·g^(-1).Furthermore,it achieves a capacity retention of 52.2%even at a high density of 5 A·g^(-1).This study first reveals the relationship between SiO crystallinity and electrochemical performance,which efficiently guides the design of high-performance SiO anodes.

Air-stable Li_(3.12)P_(0.94)Bi_(0.06)S_(3.91)I_(0.18)solid-state electrolyte with high ionic conductivity and lithium anode compatibility toward high-performance all-solid-state lithium metal batteries

Sulfide solid-state electrolytes(SSEs)with superior ionic conductivity and processability are highly promising candidates for constructing all-solid-state lithium metal batteries(ASSLMBs).However,their practical applications are limited by their intrinsic air instability and serious interfacial incompatibility.Herein,a novel glass-ceramic electrolyte Li_(3.12)P_(0.94)Bi_(0.06)S_(3.91)I_(0.18)was synthesized by co-doping Li_(3)PS_(4)with Bi and I for high-performance ASSLMBs.Owing to the strong Bi-S bonds that are thermodynamically stable to water,increased unit cell volume and Li+concentration caused by P5+substitution with Bi3+,and the in situ formed robust solid electrolyte interphase layer LiI at lithium surface,the as-prepared Li_(3.12)P_(0.94)Bi_(0.06)S_(3.91)I_(0.18)SSE achieved excellent air stability with a H2S concentration of only 0.205 cm^(3)g^(-1)(after 300 min of air exposure),outperform-ing Li_(3)PS_(4)(0.632 cm^(3)g^(-1))and the most reported sulfide SSEs,together with high ionic conductivity of 4.05 mS cm^(-1).Furthermore,the Li_(3.12)P_(0.94)Bi_(0.06)S_(3.91)I_(0.18)effectively improved lithium metal stability.With this SSE,an ultralong cyclabil-ity of 700 h at 0.1 mA cm^(-2)was realized in a lithium symmetrical cell.Moreover,the Li_(3.12)P_(0.94)Bi_(0.06)S_(3.91)I_(0.18)-based ASSLMBs with LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)cathode achieved ultrastable capacity retention rate of 95.8%after 300 cycles at 0.1 C.This work provides reliable strategy for designing advanced sulfide SSEs for commercial applications in ASSLMBs.

Chronic pulmonary bacterial infection facilitates breast cancer lung metastasis by recruiting tumor-promoting MHCII^(hi) neutrophils

Breast cancer can metastasize to various organs,including the lungs.The immune microenvironment of the organs to be metastasized plays a crucial role in the metastasis of breast cancer.Infection with pathogens such as viruses and bacteria can alter the immune status of the lung.However,the effect of chronic inflammation caused by bacteria on the formation of a premetastatic niche within the lung is unclear,and the contribution of specific immune mediators to tumor metastasis also remains largely undetermined.Here,we used a mouse model revealing that chronic pulmonary bacterial infection augmented breast cancer lung metastasis by recruiting a distinct subtype of tumor-infiltrating MHCII^(hi) neutrophils into the lung,which exhibit cancer-promoting properties.Functionally,MHCII^(hi) neutrophils enhanced the lung metastasis of breast cancer in a cell-intrinsic manner.Furthermore,we identified CCL2 from lung tissues as an important environmental signal to recruit and maintain MHCII^(hi) neutrophils.Our findings clearly link bacterial-immune crosstalk to breast cancer lung metastasis and define MHCII^(hi) neutrophils as the principal mediator between chronic infection and tumor metastasis.

Three-dimensional printing of high-mass loading electrodes for energy storage applications

Nanostructured materials afford a promising potential for many energy storage applications because of their extraordinary electrochemical properties.However,the remarkable electrochemical energy storage performance could only be harvested at a relatively low mass-loading via the traditional electrode fabrication process,and the scale of these materials into commercial-level mass-loading remains a daunting challenge because the ion diffusion kinetics deteriorates rapidly along with the increased thickness of the electrodes.Very recently,three-dimensional(3D)printing,a promising additive manufacturing technology,has been considered as an emerging method to address the aforementioned issues where the 3D printed electrodes could possess elaborately regulated architectures and rationally organized porosity.As a result,the outstanding electrochemical performance has been widely observed in energy storage devices made of 3D printed electrodes of high-mass loading.In this review,we systemically introduce the basic working principles of various 3D printing technologies and their practical applications to manufacture highmass loading electrodes for energy storage devices.Challenges and perspectives in 3D printing technologies for the construction of electrodes at the current stage are also outlined,aiming to offer some useful opinions for further development for this prosperous field.

P-band center theory guided activation of MoS_(2) basal S sites for pHuniversal hydrogen evolution

The edge S sites of thermodynamically stable 2H MoS_(2)are active for hydrogen evolution reaction(HER)but the active sites are scarce.Despite the dominance of the basal S sites,they are generally inert to HER because of the low p-band center.Herein,we reported a synergistic combination of phase engineering and NH_(4)^(+) intercalation to promote the HER performance of MoS_(2).The rational combination of 1T and 2H phases raises the p-band center of the basal S sites while the intercalated NH4+ions further optimize and stabilize the electronic band of these sites.The S sites with regulated band structures afford moderate hydrogen adsorption,thus contributing to excellent HER performance over a wide pH range.In an acid medium,this catalyst exhibits a low overpotential of 169 mV at 10 mA·cm^(−2)and Tafel slope of 39 mV·dec^(−1)with robust stability,superior to most of recently reported MoS_(2)-based non-noble catalysts.The combined use of in/ex-situ characterizations ravels that the appearance of more unpaired electrons at the Mo 4d-orbital reduces the d-band center which upshifts the p-band center of the adjacent S for essentially improved HER performance.This work provides guidelines for the future development of layered transition-metal-dichalcogenide catalysts.

Dual carbon Li-ion capacitor with high energy density and ultralong cycling life at a wide voltage window

Using the same materials for the cathode and anode in energy storage devices could greatly simplify the technological process and reduce the device cost significantly.In this paper,we assemble a dual carbon-based Li-ion capacitor with the active materials derived entirely from a single precursor,petroleum coke.For the anode,petroleum cokederived carbon(PCC)is prepared by simple ball milling and carbonization,having a massive tap density(1.80 g cm^(-3))and high electrical conductivity(11.5 S cm^(-1)).For the cathode,the raw petroleum coke is activated by KOH(petroleum cokeactivated carbon(PC-AC)sample)to achieve a well-developed pore structure to meet a rapid capacitive behavior.As a result,in addition to the robust structural stability of both the anode and cathode,the assembled dual carbon Li-ion capacitor shows a high energy density(231 W h kg^(-1)/206 W h L^(-1))and ultralong cycling life(up to 3000/10,000 cycles)at a wide voltage window.The excellent electrochemical response and simple production process make the PCC materials have great potential for practical application.

Kinetically accelerated and high-mass loaded lithium storage enabled by atomic iron embedded carbon nanofibers

Carbonaceous materials represent the dominant choice of materials for anodic lithium storage in many energy storage devices.Nevertheless,the nonpolar carbonaceous materials offer weak adsorption toward Li+that largely denies the high-rate Li+storage.Herein,the atomic Fe sites decorated carbon nanofibers(AICNFs)facilely produced by electrospinning are reported for kinetically accelerated Li+storage.Theoretical calculation reveals that the atomic Fe sites possess coordination unsaturated electronic configuration,enabling suitable bonding energy and facilitated diffusion path of Li+.As a result,the optimal structure displays a high capacitive contribution up to 95.9%at a scan rate of 2.0 mV·s^(−1).In addition,ultrahigh capacity retention of 97%is afforded after 5,000 cycles at a current density of 3 A·g^(−1).Moreover,the interlaced fiber structure enabled by electrospinning benefits structural stability and improved conductivity even at thick electrodes,thus allowing a high areal capacity of 1.76 mAh·cm−2 at a loading of 8 mg·cm−2.Because of these structure and performance merits,the lithium-ion capacitor containing the AICNF-based anode delivers a high energy density and large power density.

Intramolecular Charge Transfer-Enhanced BODIPY Photosensitizer in Photoinduced Electron Transfer and Its Application to Photoxidation under Mild Condition

Photoinduced electron transfer process is a crucial step in photooxidation to obtain synthetic chemicals. How- ever, the driving forces of electron transfer as priority in all have been rarely studied in stepwise detail. Herein, we report a series of BODIPY derivatives with an emphasis on the intramolecular charge transfer, enhancing the key step of photoinduced electron transfer process and photooxidation performances. A series of novel BODIPY photosensitizers （B-1--B-5） were prepared, wherein diethylamine amino of B-3 as charge injection group was conjugated to the 2,6-diiodo-styryl-BODIPY, and the electron transfer impetus was enhanced 1.6 times due to its more negative redox potentials. These results were also confirmed by the DFT/TDDFT calculation. Without pure oxygen, B-3 still can exhibit an exceptional performance in photoxidative aromatization of 1,4-DHP under mild condition. After irradiation for 28 rain, the conversion rate came to 98.2%.

Design and Construction of Lightweight Domain Ontology of Tectonic Geomorphology

As data size grows and computing power evolves, artificial intelligence has become one of the most important tools for assisting data-intensive scientific discoveries. The development of artificial intelligence applications in geoscience requires the understanding of enormous quantities of concepts and thus requires the organization of knowledge into a structured form, which is ontology. Compared with common-sense ontologies, the concepts in geoscience are extremely abstract and difficult to understand. It is challenging to use natural language processing technologies to build ontologies in geoscience from the bottom up. Meanwhile, applications of ontology in deep learning and data integration also reveal the importance of constructing a geoscience ontology. Because of the complexity and transdisciplinary nature, this study focuses on the field of tectonic geomorphology. Based on the understanding and experience of experts in geoscience, a top-down approach is used to construct a tectonic geomorphology ontology as part of the geoscience ontology. This research started with the proposal of a method for constructing ontologies, then built a tectonic geomorphology ontology, and finally checked, validated, and applied the ontology, covering common concepts in geoscience and dedicated concepts in tectonic geomorphology. The tectonic geomorphology ontology is an important part of the whole geoscience ontology.

Developing in situ electron paramagnetic resonance characterization for understanding electron transfer of rechargeable batteries

Electrochemical energy storage devices are pivotal in achieving“carbon neutrality”by enabling the storage of energy generated from renewable sources.To facilitate the development of these devices,it is important to gain insight into the underlying the single-/multi-electron transfer process.This can be achieved through in-time detection under operational conditions,but there are limited tools available for monitoring electron transfer under operando conditions.Electron paramagnetic resonance(EPR)is a powerful technique that can meet these expectations,as it is highly sensitive to unpaired electrons and can detect changes of paramagnetic centres.Despite the long history of in situ electrochemical EPR research,its potential has been surprisingly underutilized due to the need for strict operando cell design under special testing conditions.This review comprehensively summarizes recent efforts to understand energy storage mechanisms using in situ/operando EPR,with the aim of drawing researchers’attention to this powerful technique.After introducing the fundamental principles of EPR,we describe the critical advances made in detecting batteries using operando EPR,along with the remaining challenges and opportunities for future development of this technology in batteries.We emphasize the need for strict operando cell design and the importance of designing experiments that closely mimic real-world conditions.We believe that this review will provide innovative solutions to solve tough problems that researchers may encounter during their battery research,and ultimately contribute to the development of more efficient and sustainable energy storage devices.

Electroreduction of CO_(2) to C_(2)H_(4) Regulated by Spacing Effect:Mechanistic Insights from DFT Studies

It is crucial to construct an efficient catalyst with high activity and excellent selectivity for realizing CO_(2) electroreduction reaction(CO_(2)ER)to high-value-added chemicals,especially the C2 products.Density functional theory(DFT)provides a powerful tool for investigating the promotional effect on C2 selectivity of finely tuned catalyst structures,which is currently difficult to control using experimental techniques,such as interatomic distances.In the work,5 Cu_(2)O catalyst models are constructed with different Cu-Cu atomic spacing(d_(Cu-Cu)).The results of DFT calculations show that adjusting the d_(Cu-Cu) can effectively tailor the electronic structures of active sites,enhance catalytic activity,and improve product selectivity.Specifically,the Cu atom pair spaced at d_(Cu-Cu)=2.5Åcould optimize the adsorption configuration of*CO and enhance the binding strength of*CO,thus improving*CO adsorption energy and reducing the energy barrier of C-C coupling.The work proves the feasibility of spacing effect in enhancing the C_(2)H_(4) selectivity of CO_(2) ER and provides a new idea for the catalyst modification for other reactions of polyprotons-coupled electrons.