186 pubs · 22,561 cites · h-index 62
Experimental study demonstrates efficient single-cell protein production from non-food carbon sources by Cyberlindnera jadinii, indicating a viable pathway for sustainable nutrition.
Demonstrates a solar-driven system that converts methane and carbon dioxide into hydrogen and 4-hydroxybenzoate, suggesting a novel approach to carbon recovery.
This research demonstrates a solar-driven system converting methane and carbon dioxide into hydrogen and 4-hydroxybenzoate, suggesting new pathways for sustainable energy.
Single‐atom catalysts have emerged as cost‐effective alternatives to noble metals for the two‐electron oxygen reduction reaction (2e − ORR); however, their practical application in hydrogen peroxide (H 2 O 2 ) electrosynthesis remains limited by persistent trade‐offs among activity, selectivity, and stability. Herein, we demonstrate that synergistic integration of atomically dispersed Ni and B, N co‐dopants within a carbon matrix (Ni‐BNC) effectively regulates the 2e − ORR for efficient H 2 O 2 production. The Ni‐BNC catalyst delivers >90% Faradaic efficiency for H 2 O 2 at current densities up to ∼−400 mA cm −2 and critically maintains this high selectivity for over 50 h at −100 mA cm −2 in a flow cell, achieving a maximum production rate of 31.13 mol g −1 h −1 . In situ infrared spectroscopy and kinetic analysis revealed that B, N‐coordination facilitates electron transfer from adjacent single Ni atoms, electronically modulating the *OOH adsorption energy and lowering the kinetic barrier. The practical viability is further demonstrated in a porous solid electrolyte reactor, which continuously produces pure, salt‐free H 2 O 2 (>1,400 ppm) for 100 h. This work highlights the effectiveness of atomic‐level synergy for designing advanced electrocatalysts beyond sole active‐site engineering.
Single‐atom catalysts have emerged as cost‐effective alternatives to noble metals for the two‐electron oxygen reduction reaction (2e − ORR); however, their practical application in hydrogen peroxide (H 2 O 2 ) electrosynthesis remains limited by persistent trade‐offs among activity, selectivity, and stability. Herein, we demonstrate that synergistic integration of atomically dispersed Ni and B, N co‐dopants within a carbon matrix (Ni‐BNC) effectively regulates the 2e − ORR for efficient H 2 O 2 production. The Ni‐BNC catalyst delivers >90% Faradaic efficiency for H 2 O 2 at current densities up to ∼−400 mA cm −2 and critically maintains this high selectivity for over 50 h at −100 mA cm −2 in a flow cell, achieving a maximum production rate of 31.13 mol g −1 h −1 . In situ infrared spectroscopy and kinetic analysis revealed that B, N‐coordination facilitates electron transfer from adjacent single Ni atoms, electronically modulating the *OOH adsorption energy and lowering the kinetic barrier. The practical viability is further demonstrated in a porous solid electrolyte reactor, which continuously produces pure, salt‐free H 2 O 2 (>1,400 ppm) for 100 h. This work highlights the effectiveness of atomic‐level synergy for designing advanced electrocatalysts beyond sole active‐site engineering.
Proton exchange membrane water electrolysis (PEMWE) is a critical technology for sustainable green hydrogen production, yet its efficiency and cost are severely constrained by the kinetically sluggish kinetics and material instability of the anodic oxygen evolution reaction (OER) in acidic media. Iridium (Ir)‐ and ruthenium (Ru)‐based oxides remain the benchmark catalysts for this demanding reaction, but still face significant challenges such as the high cost and inadequate activity of Ir and the poor stability of Ru under harsh anodic conditions. In this review, recent breakthroughs in overcoming these limitations are comprehensively summarized through the strategic engineering of Ir‐ and Ru‐based electrocatalysts via single‐atom doping (SAD). Controllable synthetic methods for SAD Ir/Ru‐based catalyst design are summarized, and their underlying reaction mechanisms in the acidic OER are discussed. This single‐atom engineering method, as a promising strategy, shows exceptional potential and reliability for developing high‐performance and durable Ir/Ru‐based acidic OER catalysts, paving the way for more efficient and economically viable PEMWE systems.
Air pollutants and greenhouse gases (GHGs) pose threats to the sustainable development of human society and ecosystems. While various established techniques are available for reducing air pollutant and GHG emissions from industrial sources, they typically focus on pollutant treatment rather than conversion and utilization. Electrocatalysis is a promising technology for converting these harmful gases into valuable chemicals using renewable energy inputs under mild conditions. Air pollutants and GHGs always coexist industrially and share some similar properties. Their electrochemical conversion, which occurs through similar electron-transfer mechanisms, can therefore be achieved synergistically in a specific scenario. This review critically examines the rationality, key considerations, and practical strategies for the synergistic conversion of air pollutants and GHGs, bridging the gap between laboratory research and industrial adoption. We assess the current state of electrocatalytic technologies, covering fundamental mechanisms, electrode materials, and reactor designs. Detailed analyses of electrocatalysts for anodic, cathodic, and synergistic reactions are provided along with investigations into reactor configurations and the role of external fields in enhancing performance. By exploring the challenges and future perspectives in gas-involved electrocatalysis, this review identifies critical barriers that need to be overcome to enable large-scale industrial implementation.
The two-electron oxygen reduction reaction (2e⁻ ORR) offers a green alternative to the anthraquinone process but demands efficient catalysts. Here, we demonstrate substrate curvature as an independent design lever for 2e⁻ ORR catalysis. Cobalt phthalocyanine (CoPc) was immobilized on carbon supports of distinct geometries, i.e., planar graphene and carbon nanotubes with different diameters, to isolate the curvature effects. In alkaline flow cells, CoPc on 15 nm CNTs delivers a >15-fold higher turnover frequency than CoPc on graphene does and a maximum productivity of 73.9 mol gcat⁻¹ h⁻¹. In situ spectroscopy and density functional theory revealed curvature-induced strengthening of *OOH adsorption, lowering the barriers for H₂O₂ formation. When integrated into a 10 cm × 10 cm porous solid-electrolyte reactor, the optimal catalyst achieves >70% selectivity at 10 A and stable operation for more than 10 h. This validation positions curvature engineering as a predictable, tunable strategy for designing high-performance electrocatalysts.
This research demonstrates that platinum cluster nuclearity affects catalytic properties in different atmospheres, suggesting new strategies for catalyst optimization.
This approach combines molten-salt synthesis and in situ reduction, achieving over 90% Faradaic efficiency in CO2 reduction with exceptional stability.
Analysis reveals enhanced catalyst performance and reactor design for CO2 electroreduction to methanol, indicating potential for sustainable energy solutions.
CeOx-modified CuO catalyst shows up to 78% faradaic efficiency in CO2 reduction, suggesting improved stability and performance.
The generation of hydrogen peroxide (H 2 O 2 ), a compound with diverse applications, via the two-electron (2e − ) oxygen reduction reaction (ORR) has garnered extensive attention in both laboratory research and industrial settings. The integration of non-noble metals such as Co, Fe, Ni, Zn, Mn, Mo, or Bi into nitrogen-doped carbon (M–N–C) matrices with defined structures and active metal center sites has emerged as a promising approach for fabricating electrocatalysts for the ORR. This review uncovers the latest advancements in the development of noble metal-free single-atom electrocatalysts (M–N–C SAECs) and electrochemical reactors aimed at enhancing and stabilizing H 2 O 2 production from the 2e − ORR. Firstly, the review explores the basics of the ORR for H 2 O 2 production and the impact of electrochemical conditions. Subsequently, the synthesis strategies and characterization methods of various M–N–C SAECs are examined in depth. In addition, the structural attributes of both conventional and altered M–N–C SAECs are meticulously investigated, and the importance of engineering and optimizing reactors to elevate H 2 O 2 yields is highlighted. This review identifies the challenges and technological hurdles in bridging the gap between laboratory-scale research and practical, real-world applications.
Shows enhanced CO2 conversion efficiency in acidic conditions, suggesting improved catalyst design.
Experimental study demonstrates durable hydrogen evolution using low-loading platinum on MXene in water electrolyzers, indicating a cost-effective alternative to standard commercial catalysts.
Water electrolysis is a key process for sustainable hydrogen production. At present, the most mature and widely investigated techniques are limited to four main methods: alkaline water electrolysis, proton exchange membrane (PEM) electrolysis, anion exchange membrane (AEM) electrolysis, and solid oxide electrolysis. However, the quest for enhanced efficiency, reduced costs, and sustainable energy integration has spurred the development of unconventional design approaches for water splitting. This review explores the latest advancements in non-traditional water electrolysis techniques, including atmosphere water electrolysis, supercritical water electrolysis, external field-assisted electrolysis, electrolysis with ionic liquids, and decoupled water electrolysis. Each method offers unique benefits, such as the utilization of alternative energy sources, improved reaction kinetics, and the potential for integration with renewable energy systems. By examining the principles, advantages, and challenges of these innovative approaches, this review aims to provide a comprehensive understanding of how unconventional methods are reshaping the landscape of hydrogen production and how the insights gained from these emerging techniques can play a critical role in advancing the global transition to a hydrogen-based energy economy.
Next-generation techniques for sustainable carboxylate production generate carboxylate salts as the primary outcome. To circumvent the costly conversion of carboxylate salts to acids, we demonstrate the aqueous (non-)Kolbe electrolysis process as an alternative strategy to generate downstream value-added chemicals. Upon revealing the irreversible oxidation-induced charge transfer inhibition on the graphite anode, we propose an anion intercalation strategy to mitigate the stability problem induced by the ever-increasing overpotential. In acetate decarboxylation, we observe a high Faradaic efficiency of ~95% for non-Kolbe products (methanol and methyl acetate) at wide current densities ranging from 0.05 to 1 A cm⁻² and long-term stability at current densities of 0.15 and 0.6 A cm⁻² for 130 and 35 h, respectively. We also extended this strategy for the upgrading of long-chain carboxylates such as propionate, butyrate, and succinate. Our work provides valuable guidance for carboxylate upgrading and extendable strategy for overcoming passivation challenges in catalysis.
The electrochemical CO 2 reduction reaction (CO 2 RR) holds significant promise as a sustainable approach to address global energy challenges and reduce carbon emissions. However, achieving long‐term stability in terms of catalytic performance remains a critical hurdle for large‐scale commercial deployment. This mini‐review provides a comprehensive exploration of the key factors influencing CO 2 RR stability, encompassing catalyst design, electrode architecture, electrolyzer optimization, and operational conditions. We examine how catalyst degradation occurs through mechanisms such as valence changes, elemental dissolution, structural reconfiguration, and active site poisoning and propose targeted strategies for improvement, including doping, alloying, and substrate engineering. Additionally, advancements in electrode design, such as structural modifications and membrane enhancements, are highlighted for their role in improving stability. Operational parameters such as temperature, pressure, and electrolyte composition also play crucial roles in extending the lifespan of the reaction. By addressing these diverse factors, this review aims to offer a deeper understanding of the determinants of long‐term stability in the CO 2 RR, laying the groundwork for the development of robust, scalable technologies for efficient carbon dioxide conversion.
Bi-defect sites are highly effective for CO2 reduction (CO2RR) to formic acid, yet most catalytic surfaces predominantly feature inert, non-defective Bi sites. To overcome this limitation, herein, tensile strain is introduced on wholescale non-defective Bi sites. Under rapid thermal shock, the Bi-based metal-organic framework (Bi-MOF-TS) shows weakened Bi–O bonds and produced tiny Bi clusters. During electrochemical reduction, these clusters create numerous continuous vacancies, inducing weak tensile strain over a large range of surrounding non-defective Bi sites. This strain enhances *OHCO intermediates adsorption and substantially lowers the reaction barrier. As a result, Bi-MOF-TS achieves a faradaic efficiency above 90% across 800 mV potential range, with an impressive formate partial current density of −995 ± 93 mA cm−2. Notably, Bi-MOF-TS exhibits a high HCOOH faradaic efficiency of 96 ± 0.64% at 400 mA cm−2 in acidic electrolyte and a high single-pass carbon conversion efficiency (SPCE) of 62.0%. Additionally, a Zn-CO2 battery with Bi-MOF-TS as the cathode demonstrates a peak power density of 21.4 mW cm−2 and maintains stability over 300 cycles. A large range of inert and non-defective sites in catalysts is a primary factor impeding catalyst activity in acidic CO2 electroreduction. Here, the authors achieve high HCOOH selectivity and activity in acidic electrolyte by introducing tensile strain to activate inert sites.
High Resolution Image Download MS PowerPoint Slide Electrocatalysis, which leverages renewable electricity, has emerged as a cornerstone technology in the transition toward sustainable energy and chemical production. However, traditional electrocatalytic systems often produce mixed, impure products, necessitating costly purification. Solid-state electrolyte (SSE) reactors represent a transformative advancement by enabling the direct production of high-purity chemicals, significantly reducing purification costs and energy consumption. The versatility of SSE reactors extends to applications such as CO 2 capture and tandem reactions, aligning with the green and decentralized production paradigm. This Perspective provides a comprehensive overview of SSE reactors, discussing their principles, design innovations, and applications in producing pure chemicals─such as liquid carbon fuels, hydrogen peroxide, and ammonia─directly from CO 2 and other sources. We further explore the potential of SSE reactors in applications such as CO 2 capture and tandem reactions, highlighting their compatibility with versatile production systems. Finally, we outline future research directions for SSE reactors, underscoring their role in advancing sustainable chemical manufacturing.