Switching between C₂₊ Products and CH₄ in CO₂ Electrolysis by Tuning the Composition and Structure of Rare-Earth/Copper Catalysts

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(42), С. 23037 - 23047

Опубликована: Окт. 11, 2023

Rational regulation of the reaction pathway to produce desired products is one most significant challenges in electrochemical CO2 reduction (CO2RR). Herein, we designed a series rare-earth Cu catalysts with mixed phases. It was found that could be switched from C2+ CH4 by tuning composition and structure catalysts. Particularly at Cu/Sm atomic ratio 9/1 (Cu9Sm1-Ox), Faradaic efficiency (FE) for (FEC2+) reach 81% 700 mA cm-2 negligible CH4. However, FE (FECH4) 65% 500 over Cu1Sm9-Ox (Cu/Sm = 1/9), FEC2+ extremely low. Experiments theoretical studies indicated stable CuSm2O4 phase existed all within range 1/9. At high content, catalyst composed The small amount Sm enhance binding strength *CO facilitate C-C coupling. Conversely, Sm2O3 effectively stabilize bivalent enrich proton donors, lowering energy deep hydrogenation generate In both pathways, cooperate or phases, which induced formation different microenvironments products. This strategy also had commonality other Cu-rare-earth (La, Pr, Eu) boost CO2RR production.

Язык: Английский

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Perspectives of High‐Performance Li–S Battery Electrolytes

Advanced Functional Materials, Год журнала: 2023, Номер 34(4)

Опубликована: Окт. 22, 2023

Abstract Lithium–sulfur batteries with high energy density are considered to be one of the most promising candidates for next‐generation storage devices. Electrolyte as medium Li + transportation between electrodes, also plays a crucial role in inhibiting dissolution and diffusion lithium polysulfides Li–S batteries. The working mechanism different electrolytes is classified into “solid‐liquid‐solid” “solid‐solid” conversions. Under conversion, would inevitably face challenges such “shuttle effect” that lead poor cycle performance, under they interface mismatch limits utilization sulfur low density, while both conversion mechanisms cause uncontrollable dendrites on anode. According mechanism, can divided ether‐based, ionic liquid‐based, gel polymer electrolytes, polymer‐based solid‐state well carbonate‐based oxide/sulfide‐based conversion. Based active materials current status strategies from multiple perspectives summarized improve electrochemical hope provide comprehensive guideline toward development suitable

Язык: Английский

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Flash‐Thermal Shock Synthesis of High‐Entropy Alloys Toward High‐Performance Water Splitting

Advanced Materials, Год журнала: 2023, Номер 35(46)

Опубликована: Авг. 22, 2023

Abstract High‐entropy alloys (HEAs) provide unprecedented physicochemical properties over unary nanoparticles (NPs). According to the conventional alloying guideline (Hume–Rothery rule), however, only size‐and‐structure similar elements can be mixed, limiting possible combinations of elements. Recently, it has been reported that based on carbon thermal shocks (CTS) in a vacuum atmosphere at high temperature, ultrafast heating/cooling rates and high‐entropy environment play critical role synthesis HEAs, ruling out possibility phase separation. Since CTS requires conducting supports, Joule‐heating efficiencies rely qualities, featuring difficulties uniform heating along large area. This work proposes photo‐thermal approach as an alternative innovative synthetic method is compatible with ambient air, large‐area, remote process, free materials selection. Single flash irradiation nanofibers induced momentary high‐temperature annealing (>1800 °C within 20 ms duration, ramping/cooling >10 4 K s −1 ) successfully decorate HEA NPs up nine excellent compatibility for large‐scale (6.0 × 6.0 cm 2 nanofiber paper). To demonstrate their feasibility toward applications, senary (PtIrFeNiCoCe) are designed screened, showing activity (η overall = 777 mV) stability (>5000 cycles) water splitting, including hydrogen evolution reactions oxygen reactions.

Язык: Английский

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Yttrium‐ and nitrogen‐doped NiCo phosphide nanosheets for high‐efficiency water electrolysis

Carbon Energy, Год журнала: 2024, Номер 6(8)

Опубликована: Март 15, 2024

Abstract Engineering high‐performance and low‐cost bifunctional catalysts for H 2 (hydrogen evolution reaction [HER]) O (oxygen [OER]) under industrial electrocatalytic conditions remains challenging. Here, the first time, we use stronger electronegativity of a rare‐Earth yttrium ion (Y 3+ ) to induce in situ NiCo‐layered double‐hydroxide nanosheets from NiCo foam (NCF) treated by dielectric barrier discharge plasma NCF (PNCF), then obtain nitrogen‐doped YNiCo phosphide (N‐YNiCoP/PNCF) after phosphating process using radiofrequency nitrogen. The obtained N‐YNiCoP/PNCF has large specific surface area, rich heterointerfaces, an optimized electronic structure, inducing high activity HER (331 mV vs. 2000 mA cm −2 OER (464 reactions 1 M KOH electrolyte. X‐ray absorption spectroscopy density functional theory quantum chemistry calculations reveal that coordination number CoNi decreased with incorporation Y atoms, which much shorter bonds Ni Co ions promote long‐term stability N‐YNiCoP simulated conditions. Meanwhile, CoN‐YP 5 heterointerface formed N‐doping is active center overall water splitting. This work expands applications elements engineering electrocatalysts provides new avenue designing transition‐metal‐based renewable energy field.

Язык: Английский

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A review of chalcogenide-based perovskites as the next novel materials: Solar cell and optoelectronic applications, catalysis and future perspectives

Next Nanotechnology, Год журнала: 2024, Номер 7, С. 100102 - 100102

Опубликована: Сен. 11, 2024

Язык: Английский

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Oxophilic Tm‐Sites in MoS₂ Trigger Thermodynamic Spontaneous Water Dissociation for Enhanced Hydrogen Evolution

Advanced Energy Materials, Год журнала: 2024, Номер unknown

Опубликована: Июнь 11, 2024

Abstract 2D MoS 2 is acknowledged as a potential alternative to Pt‐based catalysts for hydrogen evolution reaction (HER) due its suitable * H adsorption energy. However, the weak water capacity of in an alkaline solution limits performance improvement toward HER. Herein, novel rare‐earth Tm single atoms decorated (Tm SAs‐MoS ) catalyst proposed, and key role SAs on enhanced HER identified. It verified that Tm‐site contributes asymmetric [Mo‐S‐Tm] unit site, which serves electron donor disturb electronic state accelerate accumulation at surrounding Mo‐S site. The obtained exhibits significantly improved activity with low overpotential 80 mV 10 mA cm −2 , robust stability good selectivity compared pure most ‐based catalysts. In situ Raman theoretical calculations prove oxophilic sites improves migration thermodynamic spontaneous dissociation interfacial O molecules during by Tm‐4f‐OH orbital overlap. Such [Tm‐S‐Mo] site allows optimal G *H location turn reaches apex volcano plot. This work expected open up new avenues design provide valuable understanding rare earth mechanisms.

Язык: Английский

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Modulation of the electronic structure of metallic bismuth catalysts by cerium doping to facilitate electrocatalytic CO₂ reduction to formate

Journal of Materials Chemistry A, Год журнала: 2024, Номер 12(13), С. 7528 - 7535

Опубликована: Янв. 1, 2024

Bi(0) metal was utilized as a CO 2 RR catalyst to achieve enhanced durability in cathodic applications. Besides, the activity effectively improved by promising strategy of electronic structure modulation through Ce doping.

Язык: Английский

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Exploring the Potential of Rare Earth Doped Carbon Dots: Concepts and Applications

Chemical Engineering Journal Advances, Год журнала: 2024, Номер 17, С. 100583 - 100583

Опубликована: Янв. 6, 2024

Carbon dots (CDs) are nanostructures containing mainly carbon atoms and abundant functional groups. With remarkable adjustable physicochemical properties, CDs have excellent hydrophilicity, photoluminescence (PL), biocompatibility, low toxicity. Although the numerous advantages make a research target for synthesizing advanced materials, some limitations pertinent must be corrected. Rare earth elements (RE) candidates doping CDs, obtaining hybrid materials called RE-CDs to optimize luminescence applicability, quantum yields. Hybrids allow combination of advantageous characteristics both RE, drastically improving their luminous magneto-optical imaging performance opening door practical technological applications. To date, no studies in literature provided in-depth analyses methods used prepare RE-CDs, characterization techniques used, challenges, critical analysis what could improved synthesis by proposing solutions. fill this gap, review initially presents detailed survey RE separately. Subsequently, addressed, as well obtainment, commonly characterizations, recent applications, from analyte detection functionality medical nanodevices. Finally, criticisms suggestions future work also discussed inspire new discoveries about potential derived RE-CDs.

Язык: Английский

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Recent Progress on Structurally Ordered Materials for Electrocatalysis

Advanced Energy Materials, Год журнала: 2021, Номер 11(37)

Опубликована: Авг. 25, 2021

Abstract Tuning material properties by modulation of the arrangement atoms is a fundamental and effective strategy in materials science. Structurally long‐range ordered are increasingly finding utility for electrocatalytic applications. Such structures can achieve unique functions that increase activity compared to corresponding electrocatalysts with disordered structure. Effective strategies designing high‐performance based on structurally presented. This review also summarizes recent progress as efficient highlights applications several representative electrochemical reactions, such as, oxygen evolution reaction, reduction hydrogen reaction. The structural features atomic framework superior performance demonstrated advanced characterization techniques (structural identification) measurements (performance evaluations), respectively. Special attention paid establishment structure‐activity relationship highlight advantages Finally, remaining challenges emerging opportunities these related proposed.

Язык: Английский

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Alloy electrocatalysts

EnergyChem, Год журнала: 2022, Номер 5(2), С. 100083 - 100083

Опубликована: Июль 22, 2022

Язык: Английский

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