A rational design of functional porous frameworks for electrocatalytic CO₂reduction reaction

Chemical Society Reviews, Год журнала: 2023, Номер 52(4), С. 1382 - 1427

Опубликована: Янв. 1, 2023

Rational design of functional porous frameworks for electrocatalytic CO 2 reduction reaction.

Язык: Английский

---

Electrocatalytic CO₂ Reduction to C₂₊ Products in Flow Cells

Advanced Materials, Год журнала: 2023, Номер 36(5)

Опубликована: Авг. 31, 2023

Abstract Electrocatalytic CO 2 reduction into value‐added fuels and chemicals by renewable electric energy is one of the important strategies to address global shortage carbon emission. Though classical H‐type electrolytic cell can quickly screen high‐efficiency catalysts, low current density limited mass transfer process essentially impede its industrial applications. The cells based on electrolyte flow system (flow cells) have shown great potential for devices, due higher density, improved local concentration, better efficiency. design optimization are significance further accelerate industrialization electrocatalytic reaction (CO RR). In this review, progress RR C 2+ products concerned. Firstly, main events in development outlined. Second, principles products, architectures, types summarized. Third, optimizing generate reviewed detail, including cathode, anode, ion exchange membrane, electrolyte. Finally, preliminary attempts, challenges, research prospects toward discussed.

Язык: Английский

---

Achievements, Challenges, and Perspectives on Nitrogen Electrochemistry for Carbon‐Neutral Energy Technologies

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(10)

Опубликована: Дек. 12, 2022

Unrestrained anthropogenic activities have severely disrupted the global natural nitrogen cycle, causing numerous energy and environmental issues. Electrocatalytic transformation is a feasible promising strategy for achieving sustainable economy. Synergistically combining multiple reactions can realize efficient renewable storage conversion, restore balance, remediate crises. Here, we provide unique aspect to discuss intriguing electrochemistry by linking three essential nitrogen-containing compounds (i.e., N2 , NH3 NO3- ) integrating four electrochemical reactions, i.e., reduction reaction (N2 RR), oxidation OR), nitrate (NO3 ammonia (NH3 OR). This minireview also summarizes acquired knowledge of rational catalyst design underlying mechanisms these interlinked reactions. We further underscore associated clean technologies nitrogen-based

Язык: Английский

---

Promoting ZIF-8-Derived Fe–N–C Oxygen Reduction Catalysts via Zr Doping in Proton Exchange Membrane Fuel Cells: Durability and Activity Enhancements

ACS Catalysis, Год журнала: 2023, Номер 13(7), С. 4221 - 4230

Опубликована: Март 13, 2023

The atomically dispersed iron site and nitrogen co-doped carbon catalysts (Fe–N–C) have demonstrated promising performance in replacing Pt toward the oxygen reduction reaction (ORR) acids for proton exchange membrane fuel cells. However, insufficient durability of Fe–N–C prohibitively hinders their practical applications. Herein, we report that co-doping Zr Fe dual metal sites into a ZIF-8-derived mesoporous exhibited significantly improved ORR. Especially, electrode assembly from ORR cathode catalyst only lost 25% voltage after 20 h continuous operation at constant current density. After an extended test up to 100 h, Zr-doped retained 40% its initial performance, superior without doping with more than 70% activity loss h. also showed activity, achieving maximum power density 0.72 W cm–2 under H2/air conditions. Extensive experimental characterization functional theory calculations suggested promoted catalytic stability are due formation Zr-based active enhanced acidic tolerance individual sites. Also, could suppress H2O2 other free radicals, thus mitigating degradation. possible Fe/Zr dual-metal sites, i.e., N2(N)–Fe–N2–Zr–N2(O2), likely intrinsic relative conventional FeNx

Язык: Английский

---

Biomass derived diverse carbon nanostructure for electrocatalysis, energy conversion and storage

Carbon, Год журнала: 2023, Номер 211, С. 118105 - 118105

Опубликована: Май 11, 2023

Язык: Английский

---

MOF@graphene nanocomposites for energy and environment applications

Composites Communications, Год журнала: 2023, Номер 45, С. 101783 - 101783

Опубликована: Ноя. 30, 2023

Язык: Английский

---

Molecular tuning for electrochemical CO2 reduction

Joule, Год журнала: 2023, Номер 7(8), С. 1700 - 1744

Опубликована: Авг. 1, 2023

Язык: Английский

---

Porous Organic Polymers‐Based Single‐Atom Catalysts for Sustainable Energy‐Related Electrocatalysis

Advanced Energy Materials, Год журнала: 2023, Номер 13(28)

Опубликована: Июнь 8, 2023

Abstract Single‐atom catalysts (SACs) have been emerging as attractive catalytic materials in electrocatalysis for sustainable energy storage and conversion. To realize the practical implementation of SACs, reliable support is highly imperative to stabilize atomically dispersed metals with strong metal–support interaction, tunable local electronic environment, favorable electron/mass transport. Thanks great designability tunability composition, structure, morphology, porous organic polymers (POPs) demonstrated grand promise appropriate platforms toward design SACs at molecular level fabrication a controlled manner. Herein, comprehensive overview recent advances elucidation general principles, effective synthesis approaches, fundamental mechanisms boosting development high‐performance POPs‐based electrocatalytic transformations provided. The authors first outline rationales using supports principles electrocatalysis, followed by discussing approaches utilizing POPs POPs‐derived nanocarbons host single‐atom metals. Then, state‐of‐the‐art their applications heterogeneous (ORR, OER, HER, CO 2 RR, NRR) are discussed, which focus on revealing structure–performance correlation mechanisms. Finally, challenges strategies associated rational suggested.

Язык: Английский

---

Nanoscale Engineering of P‐Block Metal‐Based Catalysts Toward Industrial‐Scale Electrochemical Reduction of CO₂

Advanced Energy Materials, Год журнала: 2023, Номер 13(34)

Опубликована: Июль 27, 2023

Abstract The efficient conversion of CO 2 to value‐added products represents one the most attractive solutions mitigate climate change and tackle associated environmental issues. In particular, electrochemical reduction fuels chemicals has garnered tremendous interest over last decades. Among all from reduction, formic acid is considered economically vital products. P‐block metals (especially Bi, Sn, In, Pb) have been extensively investigated recognized as catalytic materials for electroreduction formate. Despite remarkable progress, future implementation this technology at industrial‐scale hinges on ability solve remaining roadblocks. review, current research status, challenges, prospects p‐block metal‐based catalysts primarily formate are comprehensively reviewed. rational design nanostructure engineering these metal optimization their performances discussed in detail. Subsequently, recent progress development state‐of‐the‐art operando characterization techniques together with advanced cells uncover intrinsic catalysis mechanism discussed. Lastly, a perspective directions including tackling critical challenges realize its early industrial presented.

Язык: Английский

---

N and OH-Immobilized Cu₃ Clusters In Situ Reconstructed from Single-Metal Sites for Efficient CO₂ Electromethanation in Bicontinuous Mesochannels

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(2), С. 1423 - 1434

Опубликована: Янв. 3, 2024

Cu-based catalysts hold promise for electrifying CO2 to produce methane, an extensively used fuel. However, the activity and selectivity remain insufficient due lack of catalyst design principles steer complex reduction pathways. Herein, we develop a concept carbon-supported Cu by regulating active sites' atomic-scale structures engineering carbon support's mesoscale architecture. This aims provide favorable local reaction microenvironment selective pathway methane. In situ X-ray absorption Raman spectroscopy analyses reveal dynamic reconstruction nitrogen hydroxyl-immobilized Cu3 (N,OH-Cu3) clusters derived from atomically dispersed Cu–N3 sites under realistic conditions. The N,OH-Cu3 possess moderate *CO adsorption affinity low barrier hydrogenation, enabling intrinsically CO2-to-CH4 compared C–C coupling with high energy barrier. Importantly, block copolymer-derived fiber support interconnected mesopores is constructed. unique long-range mesochannels offer H2O-deficient prolong transport path CO intermediate, which could suppress hydrogen evolution favor deep toward methane formation. Thus, newly developed consisting in constructed embedded into bicontinuous achieved unprecedented Faradaic efficiency 74.2% at industry-level current density 300 mA cm–2. work explores effective concepts steering desirable pathways interfacial catalytic systems via modulating site atomic level pore architectures supports on create microenvironments.

Язык: Английский

---