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1.
Artigo em Inglês | MEDLINE | ID: mdl-34719865

RESUMO

The sluggish oxygen reaction kinetics concomitant with the high overpotentials and parasitic reactions from cathodes and solvents is the major challenge in aprotic lithium-oxygen (Li-O2 ) batteries. Herein, PtIr multipods with a low Lewis acidity of the Pt atoms are reported as an advanced cathode for improving overpotentials and stabilities. DFT calculations disclose that electrons have a strong disposition to transfer from Ir to Pt, since Pt has a higher electronegativity than Ir, resulting in a lower Lewis acidity of the Pt atoms than that on the pure Pt surface. The low Lewis acidity of Pt atoms on the PtIr surface entails a high electron density and a down-shifting of the d-band center, thereby weakening the binding energy towards intermediates (LiO2 ), which is the key in achieving low oxygen-reduction-reaction (ORR) and oxygen-evolution-reaction (OER) overpotentials. The Li-O2 cell based on PtIr electrodes exhibits a very low overall discharge/charge overpotential (0.44 V) and an excellent cycle life (180 cycles), outperforming the bulk of reported noble-metal-based cathodes.

2.
Adv Mater ; : e2105276, 2021 Nov 05.
Artigo em Inglês | MEDLINE | ID: mdl-34738668

RESUMO

Electrochemical sensors for detecting micromolecule organics are desirable for improving the perception of environmental quality and human health. However, currently, the electrochemical sensors for formaldehyde are substantially limited on the market due to the long-term unsolved problems of the low electrooxidation efficiency and CO poisoning issue of commercial Pd catalysts. Here, a 2D Cr-doped Pd metallene (Cr-Pdene) with few atomic layers is shown as an advanced catalyst for ultrasensitive and selective sensing of formaldehyde via a highly efficient formaldehyde electrooxidation. It is found that the doping of Cr into Pd metallene can efficiently optimize the electronic structure of Pd and weaken the interaction between Pd and CO, providing an anti-poisoning means to favor CO2 production and suppress CO adsorption. The Cr-Pdene-based electrochemical sensor exhibits one order of magnitude higher detection range and, especially, much higher anti-interference for formaldehyde than that of the conventional sensors. Most importantly, it is demonstrated that the Cr-Pdene can be integrated into commercializable wireless sensor networks or handheld instruments for promising applications relating to the environment, health, and food.

3.
Phys Rev Lett ; 127(18): 180501, 2021 Oct 29.
Artigo em Inglês | MEDLINE | ID: mdl-34767433

RESUMO

Scaling up to a large number of qubits with high-precision control is essential in the demonstrations of quantum computational advantage to exponentially outpace the classical hardware and algorithmic improvements. Here, we develop a two-dimensional programmable superconducting quantum processor, Zuchongzhi, which is composed of 66 functional qubits in a tunable coupling architecture. To characterize the performance of the whole system, we perform random quantum circuits sampling for benchmarking, up to a system size of 56 qubits and 20 cycles. The computational cost of the classical simulation of this task is estimated to be 2-3 orders of magnitude higher than the previous work on 53-qubit Sycamore processor [Nature 574, 505 (2019)NATUAS0028-083610.1038/s41586-019-1666-5. We estimate that the sampling task finished by Zuchongzhi in about 1.2 h will take the most powerful supercomputer at least 8 yr. Our work establishes an unambiguous quantum computational advantage that is infeasible for classical computation in a reasonable amount of time. The high-precision and programmable quantum computing platform opens a new door to explore novel many-body phenomena and implement complex quantum algorithms.

4.
Adv Mater ; : e2107638, 2021 Nov 11.
Artigo em Inglês | MEDLINE | ID: mdl-34762349

RESUMO

Li dendrite growth and unsatisfactory sulfur cathode performance are two core problems that greatly restrict the practical applications of lithium-sulfur batteries (LSBs). Here, an all-in-one design concept for Janus separator enabled by the interfacial engineering strategy is proposed to improve the performance of LSBs. At the interface of anode/separator, the thin functionalized composite layer contains the high-elastic-modulus and high-thermal-conductivity boron nitride nanosheets and oxygen group-grafted cellulose nanofibers (BNNs@CNFs), which can effectively avoid the formation of "hot spot", homogenize Li-ion flux, and suppress dendrite growth. Meanwhile, at the interface between separator and cathode, the high-density homogenously exposed Ru single atoms on the surface of reduced graphene oxide (rGO@Ru SAs) can "trap" the polysulfides and considerably reduce the activation energy to boost their conversion kinetics. Consequently, the LSBs show a high capacity of 460 mAh g-1 at 5 C and ultrastable cycling performance with an ultralow capacity decay rate of 0.046% per cycle over 800 cycles. To further demonstrate the practical prospect of our Janus separator, an assembled Li-S pouch cell using our Janus separator delivers a cell-level energy density of 310.2 Wh kg-1 . This study provides a promising strategy to simultaneously tackle the challenges facing metallic Li anode and sulfur cathode in LSBs. This article is protected by copyright. All rights reserved.

5.
Natl Sci Rev ; 8(9): nwab019, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34691734

RESUMO

The multi-metallene with an ultrahigh surface area has great potential in precise tuning of surface heterogeneous d-electronic correlation by surface strain effect for the distinctive surface electronic structure, which is a brand new class of promising 2D electrocatalyst for sustainable energy device application. However, achieving such an atomically thin multi-metallene still presents a great challenge. Herein, we present a new synthetic method for an atomic-level palladium-iridium (PdIr) bimetallene with an average thickness of only ∼1.0 nm for achieving superior catalysis in the hydrogen evolution reaction (HER) and the formic acid oxidation reaction (FAOR). The curved PdIr bimetallene presents a top-ranked high electrochemical active area of 127.5 ± 10.8 m2 gPd+Ir -1 in the reported noble alloy materials, and exhibits a very low overpotential, ultrahigh activity and improved stability for HER and FAOR. DFT calculation reveals that the PdIr bimetallene herein has a unique lattice tangential strain, which can induce surface distortion while concurrently creating a variety of concave-convex featured micro-active regions formed by variously coordinated Pd sites agglomeration. Such a strong strain effect correlates the abnormal on-site active 4d10-t2g-orbital Coulomb correlation potential and directly elevates orbital-electronegativity exposure within these active regions, resulting in a preeminent barrier-free energetic path for significant enhancement of FAOR and HER catalytic performance.

6.
Artigo em Inglês | MEDLINE | ID: mdl-34590399

RESUMO

The development of high-performance anode materials for potassium-based energy storage devices with long-term cyclability requires combined innovations from rational material design to electrolyte optimization. A three-dimensional K+ -pre-intercalated Ti3 C2 Tx MXene with enlarged interlayer distance was constructed for efficient electrochemical potassium-ion storage. We found that the optimized solvation structure of the concentrated ether-based electrolyte leads to the formation of a thin and inorganic-rich solid electrolyte interphase (SEI) on the K+ -pre-intercalated Ti3 C2 Tx electrode, which is beneficial for interfacial stability and reaction kinetics. As a proof of concept, 3D K+ -Ti3 C2 Tx //activated carbon (AC) potassium-ion hybrid capacitors (PIHCs) were assembled, which exhibited promising electrochemical performances. These results highlight the significant roles of both rational structure design and electrolyte optimization for highly reactive MXene-based anode materials in energy storage devices.

7.
Angew Chem Int Ed Engl ; 60(43): 23388-23393, 2021 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-34370386

RESUMO

PtSe2 is a typical noble metal dichalcogenide (NMD) that holds promising possibility for next-generation electronics and photonics. However, when applied in hydrogen evolution reaction (HER), it exhibits sluggish kinetics due to the insufficient capability of absorbing active species. Here, we construct PtSe2 /Pt heterointerface to boost the reaction dynamics of PtSe2 , enabled by an in situ electrochemical method. It is found that Se vacancies are induced around the heterointerface, reducing the coordination environment. Correspondingly, the exposed Pt atoms at the very vicinity of Se vacancies are activated, with enhanced overlap with H 1s orbital. The adsorption of H. intermediate is thus strengthened, achieving near thermoneutral free energy change. Consequently, the as-prepared PtSe2 /Pt exhibits extraordinary HER activity even superior to Pt/C, with an overpotential of 42 mV at 10 mA cm-2 and a Tafel slope of 53 mV dec-1 . This work raises attention on NMDs toward HER and provides insights for the rational construction of novel heterointerfaces.

8.
Adv Mater ; 33(41): e2103762, 2021 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-34423488

RESUMO

A crucial issue restricting the application of direct alcohol fuel cells (DAFCs) is the low activity of Pt-based electrocatalysts for alcohol oxidation reaction caused by the reaction intermediate (CO*) poisoning. Herein, a new strategy is demonstrated for making a class of sub-monolayer YOx /MoOx -surface co-decorated ultrathin platinum nanowires (YOx /MoOx -Pt NWs) to effectively eliminate the CO poisoning for enhancing methanol oxidation electrocatalysis. By adjusting the amounts of YOx and MoOx decorated on the surface of ultrathin Pt NWs, the optimized 22% YOx /MoOx -Pt NWs achieve a high specific activity of 3.35 mA cm-2 and a mass activity of 2.10 A mgPt -1 , as well as the enhanced stability. In situ Fourier transform infrared (FTIR) spectroscopy and CO stripping studies confirm the contribution of YOx and MoOx to anti-CO poisoning ability of the NWs. Density functional theory (DFT) calculations further reveal that the surface Y and Mo atoms with oxidation states allow COOH* to bind the surface through both the carbon and oxygen atoms, which can lower the free energy barriers for the oxidation of CO* into COOH*. The optimal NWs also show the superior activities toward the electro-oxidation of ethanol, ethylene glycol, and glycerol.

9.
J Am Chem Soc ; 143(29): 10822-10827, 2021 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-34279921

RESUMO

The electrosynthesis of high-value-added multicarbon compounds coupled with hydrogen production is an efficient way to achieve carbon neutrality; however, the lack of effective bifunctional catalysts in electrosynthesis largely hinders its development. Herein, we report the first example on the highly efficient electrosynthesis of high-value-added 1,1-diethoxyethane (DEE) at the anode and high-purity hydrogen at the cathode using 1 nm PtIr nanowires (NWs) as the bifunctional catalysts. We demonstrate that the cell using 1 nm PtIr nanowires as the bifunctional catalysts can achieve a reported lowest voltage of 0.61 V to reach the current density of 10 mA cm-2, much lower than those of the Pt NWs (0.85 V) and commercial Pt/C (0.86 V), and also can have the highest Faraday efficiencies of 85% for DEE production and 94.0% for hydrogen evolution in all the reported electrosynthesis catalysts. The in situ infrared spectroscopy study reveals that PtIr NWs can facilitate the activation of O-H and C-H bonds in ethanol, which is important for the formation of acetaldehyde intermediate, and finally DEE. In addition, the cell using PtIr NWs as bifunctional catalysts exhibits excellent stability by showing almost no obvious decrease in the Faraday efficiency of the DEE production.

10.
Phys Rev Lett ; 127(2): 020602, 2021 Jul 09.
Artigo em Inglês | MEDLINE | ID: mdl-34296924

RESUMO

We experimentally study the ergodic dynamics of a 1D array of 12 superconducting qubits with a transverse field, and identify the regimes of strong and weak thermalization with different initial states. We observe convergence of the local observable to its thermal expectation value in the strong-thermalizaion regime. For weak thermalization, the dynamics of local observable exhibits an oscillation around the thermal value, which can only be attained by the time average. We also demonstrate that the entanglement entropy and concurrence can characterize the regimes of strong and weak thermalization. Our work provides an essential step toward a generic understanding of thermalization in quantum systems.

11.
Adv Mater ; 33(36): e2102576, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34296795

RESUMO

Atomically dispersed metal catalysts with well-defined structures have been the research hotspot in heterogeneous catalysis because of their high atomic utilization efficiency, outstanding activity, and selectivity. Dual-atomic-site catalysts (DASCs), as an extension of single-atom catalysts (SACs), have recently drawn surging attention. The DASCs possess higher metal loading, more sophisticated and flexible active sites, offering more chance for achieving better catalytic performance, compared with SACs. In this review, recent advances on how to design new DASCs for enhancing energy catalysis will be highlighted. It will start with the classification of marriage of two kinds of single-atom active sites, homonuclear DASCs and heteronuclear DASCs according to the configuration of active sites. Then, the state-of-the-art characterization techniques for DASCs will be discussed. Different synthetic methods and catalytic applications of the DASCs in various reactions, including oxygen reduction reaction, carbon dioxide reduction reaction, carbon monoxide oxidation reaction, and others will be followed. Finally, the major challenges and perspectives of DASCs will be provided.

12.
ACS Appl Mater Interfaces ; 13(28): 32997-33005, 2021 Jul 21.
Artigo em Inglês | MEDLINE | ID: mdl-34251788

RESUMO

Because of the favorable mass transport and increased available active sites, the rational design and preparation of porous carbon structures are essential but still challenging. Herein, a novel and facile supramolecular anchoring strategy was developed to achieve the embedding of ruthenium (Ru) nanoparticles in N-doped mesoporous carbon nanospheres through pyrolyzing the precursor formed by coordination assembly between metal ions and zinc gluconate (G(Zn)). Featuring rich hydroxyl groups, the G(Zn) can effectively chelate Ru3+ via metal-oxygen bonds to form 3D supramolecular nanospheres, and meanwhile, mesopores in carbon nanospheres were expanded after subsequent pyrolysis thanks to the volatilization of zincic species at high temperature. As a demonstration, the best-performing catalyst displayed extraordinary activity for the hydrogen evolution reaction (HER) with a small overpotential of 43 mV versus reversible hydrogen electrode (vs RHE) at 10 mA/cm2 and a Tafel slope of 39 mV/dec, which was superior to that of commercial Pt/C in alkaline medium. Theoretical calculations revealed that the catalytic activity was significantly promoted by the strong electronic coupling between Ru nanoparticles and N-doped porous carbon, which increased the electron transfer capability and facilitated the adsorption and dissociation of H2O to realize an efficient HER.

13.
Nat Commun ; 12(1): 4412, 2021 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-34285217

RESUMO

Organic-inorganic lead halide perovskites are a new class of semiconductor materials with great potential in photocatalytic hydrogen production, however, their development is greatly plagued by their low photocatalytic activity, instability of organic component and lead toxicity in particular. Herein, we report an anti-dissolution environmentally friendly Cs2SnI6 perovskite anchored with a new class of atomically dispersed Pt-I3 species (PtSA/Cs2SnI6) for achieving the highly efficient photocatalytic hydrogen production in HI aqueous solution at room temperature. Particularly, we discover that Cs2SnI6 in PtSA/Cs2SnI6 has a greatly enhanced tolerance towards HI aqueous solution, which is very important for achieving excellent photocatalytic stability in perovskite-based HI splitting system. Remarkably, the PtSA/Cs2SnI6 catalyst shows a superb photocatalytic activity for hydrogen production with a record turnover frequency of 70.6 h-1 per Pt, about 176.5 times greater than that of Pt nanoparticles supported Cs2SnI6 perovskite, along with superior cycling durability. Charge-carrier dynamics studies in combination with theory calculations reveal that the dramatically boosted photocatalytic performance on PtSA/Cs2SnI6 originates from both unique coordination structure and electronic property of Pt-I3 sites, and strong metal-support interaction effect that can not only greatly promote the charge separation and transfer, but also substantially reduce the energy barrier for hydrogen production. This work opens a new way for stimulating more research on perovskite composite materials for efficient hydrogen production.

14.
Nano Lett ; 21(13): 5774-5781, 2021 07 14.
Artigo em Inglês | MEDLINE | ID: mdl-34187162

RESUMO

The high-valence metal catalysts show extraordinary talent in various electrochemical reactions. However, there is no facile method to synthesize high-valence noble metal-based materials. Herein, we synthesized the different high valence noble metal M-incorporated PdCu nanoparticles (M = Ir, Ru, Rh) by the assistant of Fe3+ and exhibit excellent performance for water electrolysis. In 0.1 M KOH, the OER and HER mass activities of Ir16-PdCu/C were 50.5 and 16.5 times as much as PdCu/C, and achieved a current density of 10 mA cm-2 at 1.63 V when worked for overall water splitting. DFT calculation revealed that the incorporating of high valence Ir could optimize the binding energy of the intermediate products, and promote the evolution of oxygen and hydrogen. Ex situ XPS shows that the huge amount of oxidized Ir (V) formed in OER could promote the formation of O-O bonds.


Assuntos
Eletrólise , Água , Catálise , Hidrogênio , Oxigênio
15.
Adv Mater ; 33(31): e2100272, 2021 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-34165842

RESUMO

The fast and reversible potassiation/depotassiation of anode materials remains an elusive yet intriguing goal. Herein, a class of the P-doping-induced orthorhombic CoTe2 nanowires with Te vacancy defects supported on MXene (o-P-CoTe2 /MXene) is designed and prepared, taking advantage of the synergistic effects of the conductive o-P-CoTe2 arrays with rich Te vacancy defects and the elastic MXene sheets with self-autoadjustable function. Consequently, the o-P-CoTe2 /MXene superstructure exhibits boosted potassium-storage performance, in terms of high reversible capacity (373.7 mAh g-1 at 0.2 A g-1 after 200 cycles), remarkable rate capability (168.2 mAh g-1 at 20 A g-1 ), and outstanding long-term cyclability (0.011% capacity decay per cycle over 2000 cycles at 2 A g-1 ), representing the best performance in transition-metal-dichalcogenides-based anodes to date. Impressively, the flexible full battery with o-P-CoTe2 /MXene anode achieves a satisfying energy density of 275 Wh kg-1 and high bending stability. The kinetics analysis and first-principles calculations reveal superior pseudocapacitive property, high electronic conductivity, and favorable K+ ion adsorption and diffusion capability, corroborating fast K+ ion storage. Especially, ex situ characterizations confirm o-P-CoTe2 /MXene undergoes reversible evolutions of initially proceeding with the K+ ion insertion, followed by the conversion reaction mechanism.

16.
Science ; 372(6545): 948-952, 2021 05 28.
Artigo em Inglês | MEDLINE | ID: mdl-33958483

RESUMO

Quantum walks are the quantum mechanical analog of classical random walks and an extremely powerful tool in quantum simulations, quantum search algorithms, and even for universal quantum computing. In our work, we have designed and fabricated an 8-by-8 two-dimensional square superconducting qubit array composed of 62 functional qubits. We used this device to demonstrate high-fidelity single- and two-particle quantum walks. Furthermore, with the high programmability of the quantum processor, we implemented a Mach-Zehnder interferometer where the quantum walker coherently traverses in two paths before interfering and exiting. By tuning the disorders on the evolution paths, we observed interference fringes with single and double walkers. Our work is a milestone in the field, bringing future larger-scale quantum applications closer to realization for noisy intermediate-scale quantum processors.

17.
Nanoscale ; 13(20): 9315-9321, 2021 May 27.
Artigo em Inglês | MEDLINE | ID: mdl-33983347

RESUMO

Developing an efficient single component photocatalyst for overall water splitting under visible-light irradiation is extremely challenging. Herein, we report a metal-free graphitic carbon nitride (g-CxN4)-based nanosheet photocatalyst (x = 3.2, 3.6, or 3.8) with melem rings conjugated by Schiff-base bonds (N[double bond, length as m-dash]C-C[double bond, length as m-dash]N). The presence of the conjugated Schiff-base bond tunes the band gap of g-CxN4 and, more importantly, serves as an electron sink to suppress electron-hole pair recombination. The projected density of states (PDOS) calculations suggest that the melem ring and Schiff-base bond act as oxidizing and reducing centers, respectively, for photocatalytic water splitting. As a result, g-CxN4, in particular g-C3.6N4, can catalyze overall water splitting without the need for any co-catalyst or sacrificial donor. Under visible light (>420 nm wavelength) irradiation, g-C3.6N4 catalyzes the overall water splitting with H2 and O2 generation rates of 75.0 and 36.3 µmol h-1 g-1, respectively. g-C3.6N4 is the most efficient single-component photocatalyst ever reported for overall water splitting. Our studies demonstrate a new approach for tuning the bandgap and the electronic structure of graphitic carbon nitride for maximizing its photocatalytic performance for water splitting, which will be important for hydrogen generation and for energy applications.

18.
Nano Lett ; 21(10): 4262-4269, 2021 May 26.
Artigo em Inglês | MEDLINE | ID: mdl-33962514

RESUMO

Single-atom catalysts (SACs) exhibit great potential in heterogeneous catalysis. However, the achievement of obtaining high-loading SACs remains a bottleneck. Herein, we first demonstrate a unique gas-migration, trapping, and emitting strategy for building a kind of Cd-based SAC for CO2 reduction (CO2RR). The gas-migration and trapping processes (≤750 °C) endows the material with an ultrahigh Cd loading amount of 30.3 wt %, while the emitting process can facilely modulate the loading amount from 30.3 to 1.4 wt %. For the CO2RR, the Cd-NC SACs with a loading amount of 18.4 wt % exhibits the maximum Faraday efficiency of 91.4% for CO at -0.728 V. The operando infrared spectroscopy studies prove the presence of main intermediates *COO-, *COOH, and *CO on Cd-NC-5M SACs during the catalytic process, indicating that the CO2RR follows the proton-decoupled electron-transfer mechanism. Density functional theory simulations reveal that the Cd-N4 structure reduces the Gibbs free energy of the rate-determining step (the hydrogenation step of *COOH).

19.
Nano Lett ; 21(11): 4861-4867, 2021 Jun 09.
Artigo em Inglês | MEDLINE | ID: mdl-34044536

RESUMO

The main challenge for lithium-oxygen (Li-O2) batteries is their sluggish oxygen evolution reaction (OER) kinetics and high charge overpotentials caused by the poorly conductive discharge products of lithium peroxide (Li2O2). In this contribution, the cesium lead bromide perovskite (CsPbBr3) nanocrystals were first employed as a high-performance cathode for Li-O2 batteries. The battery with a CsPbBr3 cathode can exhibit the lowest charge overpotential of 0.5 V and the best cycling performance of 400 cycles among all the reported perovskite-based Li-O2 cells, which represents a new benchmark. Most importantly, the density functional theory (DFT) calculations further prove that the rate limitation step during OER processes is the decomposition of LiO2 to form O2 and Li+, and the weak adsorption strength between CsPbBr3 surfaces and LiO2 results in a low charge overpotential for the CsPbBr3-based Li-O2 battery. This work first demonstrates the good potential of CsPbBr3 for application in metal-air batteries.

20.
ACS Appl Mater Interfaces ; 13(15): 17668-17676, 2021 Apr 21.
Artigo em Inglês | MEDLINE | ID: mdl-33830722

RESUMO

Potassium-ion batteries (KIBs) are emerging as the prospective alternatives to lithium-ion batteries in energy storage systems owing to the sufficient resources and relatively low cost of K-related materials. However, serious volume expansion and low specific capacity are found in most materials systems resulting from the large intrinsic radius of K+. Herein, SnS2 nanosheets anchored on nitrogen and sulfur co-doped MXene (SnS2 NSs/MXene) are creatively designed as advanced anode materials for KIBs. SnS2 NSs/MXene with a unique hierarchical structure can not only provide fast transmission channels for K+ but also avoid the accumulation of K+ and volume expansion. These novel features make SnS2 NSs/MXene electrodes exhibit a superior reversible specific capacity of 342.4 mA h g-1 under 50 mA g-1. Also, they maintain 206.1 mA h g-1 at an even higher current density of 0.5 A g-1 over 800 cycles almost without capacity decay. Moreover, the multistep alloying reaction mechanism of SnS2 NSs/MXene composites and K+ is revealed by the ex situ X-ray diffraction measurement. In addition, the density functional theory calculations confirm the existence of Ti-S bonds between SnS2 nanosheets and MXene, which significantly enhance the structural stability and cycling electrochemical performance of SnS2 NSs/MXene composites.

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