Electrochemical reduction of carbon dioxide to multicarbon (C₂₊) products: challenges and perspectives

Energy & Environmental Science, Год журнала: 2023, Номер 16(11), С. 4714 - 4758

Опубликована: Янв. 1, 2023

This review analyzes advanced catalysts and C 2+ synthesis mechanisms based on theoretical explorations in situ / operando characterizations. Triphasic interface optimization is discussed for the potential of industry-compatible stability.

Язык: Английский

---

Regulating reconstruction of oxide-derived Cu for electrochemical CO ₂ reduction toward n-propanol

Science Advances, Год журнала: 2023, Номер 9(43)

Опубликована: Окт. 27, 2023

Oxide-derived copper (OD-Cu) is the most efficient and likely practical electrocatalyst for CO 2 reduction toward multicarbon products. However, inevitable but poorly understood reconstruction from pristine state to working of OD-Cu under strong conditions largely hinders rational construction catalysts products, especially C 3 products like n-propanol. Here, we simulate CuO Cu O into their derived by molecular dynamics, revealing that CuO-derived (CuOD-Cu) intrinsically has a richer population undercoordinated sites higher surficial atom density than counterpart O-derived (Cu OD-Cu) because vigorous oxygen removal. In situ spectroscopes disclose coordination number CuOD-Cu considerably lower OD-Cu, enabling fast kinetics reaction strengthened binding *C intermediate(s). Benefiting rich sites, achieves remarkable n-propanol faradaic efficiency up ~17.9%, whereas dominantly generates formate.

Язык: Английский

---

Localized surface plasmon resonance-induced bidirectional electron transfer of formic acid adsorption for boosting photocatalytic hydrogen production on Ni/TiO2

Chemical Engineering Journal, Год журнала: 2024, Номер 482, С. 148942 - 148942

Опубликована: Янв. 20, 2024

Язык: Английский

---

Selectively nucleotide‐derived RuP on N,P‐codoped carbon with engineered mesopores for energy‐efficient hydrogen production assisted by hydrazine oxidation

SusMat, Год журнала: 2024, Номер 4(1), С. 166 - 177

Опубликована: Фев. 1, 2024

Abstract Integrating hydrogen evolution reaction (HER) with hydrazine oxidation (HzOR) has an encouraging prospect for the energy‐saving production, demanding high‐performance bifunctional HER/HzOR electrocatalyst. Ruthenium phosphide/doped carbon composites have exhibited superior activity toward multiple electrocatalytic reactions. To explore decent water‐soluble precursors containing both N and P elements is highly attractive to facilely prepare metal composites. Herein, as one kind ecofriendly biomolecules, adenine nucleotide was first employed selectively fabricate pure RuP nanoparticles embedded into porous N,P‐codoped carbons (RuP/PNPC) a straightforward “mix‐and‐pyrolyze” approach. The newly prepared RuP/PNPC only requires 4.0 −83.0 mV at 10 mA/cm 2 separately in alkaline HER HzOR, outperforming most of reported electrocatalysts, together outstanding neutral performance. Furthermore, two‐electrode overall splitting exhibit significant power‐efficiency superiority corresponding water voltage difference larger than V, which can be also easily driven by fuel cells solar considerable H generation. Our report innovates N‐ P‐bearing effortlessly synthesize high‐quality RuP/doped composite catalysts, potential universal platform phosphide‐related functional materials.

Язык: Английский

---

Boosting Solar‐Driven CO₂ Conversion to Ethanol via Single‐Atom Catalyst with Defected Low‐Coordination Cu‐N₂ Motif

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(31)

Опубликована: Май 18, 2024

Cu-based catalysts have been shown to selectively catalyze CO

Язык: Английский

---

Modulating structural oxygen/crystallinity enables ambient cascade photo‐upgrading of biomass saccharides to lactic acid

Carbon Energy, Год журнала: 2025, Номер unknown

Опубликована: Янв. 7, 2025

Abstract Photocatalytic transformation of biomass into biofuels and value‐added chemicals is great significance for carbon neutrality. Metal‐free nitride has extensive applications but with almost no absorption utilization near‐infrared light, accounting 50% sunlight. Here, a molten salt‐assisted in‐plane “stitching” interlayer “cutting” protocol developed constructing highly crystalline catalyst containing structural oxygen (HC‐CN). HC‐CN efficient the photothermal cascade biomass‐derived glucose lactic acid (LA) an unprecedented yield (94.3%) at 25°C under full‐spectrum light irradiation within 50 min, which also applicable to quantitatively photo‐upgrading various saccharides. Theoretical calculations expound that light‐induced glucose‐to‐catalyst charge transfer can activate C β –H bond promote rate‐determining step intramolecular hydrogen shift in glucose‐to‐fructose isomerization. Meanwhile, introduced not only facilitate local electric field formation achieve rapid transport/separation regulate selective •O 2 − generation oriented C3–C4 cleavage fructose narrow energy band gap broaden range HC‐CN, contributing enhanced LA production without exogenous heating. Moreover, recyclable exhibits negligible environmental burden low consumption, as disclosed by life cycle assessment. Tailored construction adsorption versatile reaction sites provides reference implementing multi‐step organic conversion processes mild conditions.

Язык: Английский

---

Copper isolated sites on MXene for efficiency aniline synthesis utilizing H2S as a hydrogen source

Chemical Engineering Science, Год журнала: 2025, Номер unknown, С. 121327 - 121327

Опубликована: Фев. 1, 2025

Язык: Английский

---

Photoenzymatic CO₂ Reduction Dominated by Collaborative Matching of Linkage and Linker in Covalent Organic Frameworks

Journal of the American Chemical Society, Год журнала: 2023, Номер 146(1), С. 586 - 598

Опубликована: Дек. 18, 2023

Artificial photoenzymatic systems based on covalent organic frameworks (COFs) provide an interesting platform for converting CO2 to value-added fuels. However, the dual roles of COFs as photocatalysts and enzyme hosts showcase contradictory preferences structures, which poses a great challenge their rational design. Herein, we report collaborative matching linkages linkers in ability exert both photocatalytic activity loading, has been neglected until now. The linkage-dependent linker regulation pattern was elucidated, optimal match showed record-breaking apparent quantum efficiency at 420 nm cofactor regeneration 13.95% with high turnover frequency 5.3 mmol g–1 h–1, outperforming other reported crystalline framework photocatalysts. Moreover, theoretical calculations experiments revealed mechanism underlying effects linkage exciton dissociation charge migration photocatalysis. This newfound understanding enabled construction photoactivity large pores closer size formate dehydrogenase, achieving loading capacity suitable confinement effect. Remarkably, artificial system constructed according linkage-linker exhibited highly efficient reduction, yielding formic acid specific 1.46 catalyst h–1 good reusability, paving way sustainable conversion driven by visible light.

Язык: Английский

---

Atomic Dispersed Hetero-Pairs for Enhanced Electrocatalytic CO2 Reduction

Nano-Micro Letters, Год журнала: 2023, Номер 16(1)

Опубликована: Ноя. 6, 2023

Abstract Electrochemical carbon dioxide reduction reaction (CO 2 RR) involves a variety of intermediates with highly correlated and ad-desorption energies, hindering optimization the catalytic activity. For example, increasing binding *COOH to active site will generally increase *CO desorption energy. Breaking this relationship may be expected dramatically improve intrinsic activity CO RR, but remains an unsolved challenge. Herein, we addressed conundrum by constructing unique atomic dispersed hetero-pair consisting Mo-Fe di-atoms anchored on N-doped carrier. This system shows unprecedented RR TOF 3336 h −1 , high selectivity toward production, Faradaic efficiency 95.96% at − 0.60 V excellent stability. Theoretical calculations show that diatomic sites increased intermediate adsorption energy bridging intermediates. At same time, d-d orbital coupling in di-atom results electron delocalization facilitates Thus, undesirable correlation between these steps is broken. work provides promising approach, specifically use di-atoms, for breaking unfavorable relationships based understanding mechanisms scale.

Язык: Английский

---

Strategies to achieve effective nitrogen activation

Carbon Energy, Год журнала: 2024, Номер 6(5)

Опубликована: Фев. 23, 2024

Abstract Ammonia serves as a crucial chemical raw material and hydrogen energy carrier. Aqueous electrocatalytic nitrogen reduction reaction (NRR), powered by renewable energy, has attracted tremendous interest during the past few years. Although some achievements have been revealed in aqueous NRR, significant challenges also identified. The activity selectivity are fundamentally limited activation competitive evolution. This review focuses on hurdles of delves into complementary strategies, including materials design system optimization (reactor, electrolyte, mediator). Then, it introduces advanced interdisciplinary technologies that recently emerged for using high‐energy physics such plasma triboelectrification. With better understanding corresponding mechanisms coming years, these potential to be extended further applications. provides insight stability different systems. We then recommend rigorous detailed protocol investigating NRR performance highlight several research directions this exciting field, coupling with applications, situ/operando characterizations, theoretical calculations.

Язык: Английский

---