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Rational design efficient transition metal-based electrocatalysts for oxygen evolution reaction (OER) is critical for water splitting. However, industrial water-alkali electrolysis requires large current densities at low overpotentials, always limited by intrinsic activity. Herein, we report hierarchical bimetal nitride/hydroxide (NiMoN/NiFe LDH) array as model catalyst, regulating the electronic states and tracking the relationship of structure-activity. As-activated NiMoN/NiFe LDH exhibits the industrially required current density of 1000 mA cm −2 at overpotential of 266 mV with 250 h stability for OER. Especially, in-situ electrochemical spectroscopic reveals that heterointerface facilitates dynamic structure evolution to optimize electronic structure. Operando electrochemical impedance spectroscopy implies accelerated OER kinetics and intermediate evolution due to fast charge transport. The OER mechanism is revealed by the combination of theoretical and experimental studies, indicating as-activated NiMoN/NiFe LDH follows lattice oxygen oxidation mechanism with accelerated kinetics. This work paves an avenue to develop efficient catalysts for industrial water electrolysis via tuning electronic states. Rational design of efficient electrocatalysts for oxygen evolution reaction is critical for water-alkali electrolysis. Here, the authors fabricate a NiMoN/NiFe layered double hydroxide and show the accelerated oxygen evolution kinetics are due to the heterointerface.

An inorganic cluster replicates many of the structural aspects of the complex that photosplits water and powers photosynthesis [Also see Report by Zhang et al. ] The oxygen evolution complex (OEC) in photosystem II (PSII) catalyzes the photosplitting of water. The resulting electrons and protons are then ultimately used to create adenosine triphosphate to convert carbon dioxide (CO 2 ) into organic compounds. An artificial catalyst that mimics the small inorganic OEC cluster within the much larger PSII enzyme could be used to create fuels such as hydrogen from water via sunlight ( 1 ). Although tremendous efforts have been spent on artificial photosynthesis systems ( 2 ), synthetic water oxidation catalysts that closely mimic the structure and function of OEC in PSII have been very limited. Now, on page 690 of this issue, Zhang et al. ( 3 ) describe the closest structural mimic of the OEC in PSII reported to date.

Electrocatalytic urea synthesis is an emerging alternative technology to the traditional energy-intensive industrial urea synthesis protocol. Novel strategies are urgently needed to promote the electrocatalytic C–N coupling process and inhibit the side reactions. Here, we report a CuWO 4 catalyst with native bimetallic sites that achieves a high urea production rate (98.5 ± 3.2 μg h −1  mg −1 cat ) for the co-reduction of CO 2 and NO 3 − with a high Faradaic efficiency (70.1 ± 2.4%) at −0.2 V versus the reversible hydrogen electrode. Mechanistic studies demonstrated that the combination of stable intermediates of *NO 2 and *CO increases the probability of C–N coupling and reduces the potential barrier, resulting in high Faradaic efficiency and low overpotential. This study provides a new perspective on achieving efficient urea electrosynthesis by stabilizing the key reaction intermediates, which may guide the design of other electrochemical systems for high-value C–N bond-containing chemicals. Electrocatalytic urea synthesis is an emerging alternative technology to the traditional urea synthesis protocol. Here, a CuWO 4 catalyst with native bimetallic sites achieves efficient co-reduction of carbon dioxide and nitrate to urea by stabilizing intermediates of *NO 2 and *CO for C–N coupling.

First-row transition metal-based catalysts have been developed for the oxygen evolution reaction (OER) during the past years, however, such catalysts typically operate at overpotentials ( η ) significantly above thermodynamic requirements. Here, we report an iron/nickel terephthalate coordination polymer on nickel form ( NiFeCP/NF ) as catalyst for OER, in which both coordinated and uncoordinated carboxylates were maintained after electrolysis. NiFeCP/NF exhibits outstanding electro-catalytic OER activity with a low overpotential of 188 mV at 10 mA cm −2 in 1.0 KOH, with a small Tafel slope and excellent stability. The pH-independent OER activity of NiFeCP/NF on the reversible hydrogen electrode scale suggests that a concerted proton-coupled electron transfer (c-PET) process is the rate-determining step (RDS) during water oxidation. Deuterium kinetic isotope effects, proton inventory studies and atom-proton-transfer measurements indicate that the uncoordinated carboxylates are serving as the proton transfer relays, with a similar function as amino acid residues in photosystem II (PSII), accelerating the proton-transfer rate. Proton-coupled electron transfer (PCET) process is very important for water oxidation catalysis. Here, the authors introduced uncoordinated carboxylate in the second-coordination-sphere of Ni-Fe coordination polymer catalyst as an internal base to promote the water oxidation kinetics by such PCET process.

Rational design of the catalysts is impressive for sustainable energy conversion. However, there is a grand challenge to engineer active sites at the interface. Herein, hierarchical transition bimetal oxides/sulfides heterostructure arrays interacting two-dimensional MoO x /MoS 2 nanosheets attached to one-dimensional NiO x /Ni 3 S 2 nanorods were fabricated by oxidation/hydrogenation-induced surface reconfiguration strategy. The NiMoO x /NiMoS heterostructure array exhibits the overpotentials of 38 mV for hydrogen evolution and 186 mV for oxygen evolution at 10 mA cm −2 , even surviving at a large current density of 500 mA cm −2 with long-term stability. Due to optimized adsorption energies and accelerated water splitting kinetics by theory calculations, the assembled two-electrode cell delivers the industrially relevant current densities of 500 and 1000 mA cm −2 at record low cell voltages of 1.60 and 1.66 V with excellent durability. This research provides a promising avenue to enhance the electrocatalytic performance of the catalysts by engineering interfacial active sites toward large-scale water splitting. While water splitting is an appealing carbon-neutral strategy for renewable energy generation, there is a need to develop new active, cost-effective catalysts. Here, authors prepare a nickel-molybdenum oxide/sulfide heterojunctions as bifunctional H 2 and O 2 evolution electrocatalysts.

Electrochemical water splitting requires efficient water oxidation catalysts to accelerate the sluggish kinetics of water oxidation reaction. Here, we report a promisingly dendritic core-shell nickel-iron-copper metal/metal oxide electrode, prepared via dealloying with an electrodeposited nickel-iron-copper alloy as a precursor, as the catalyst for water oxidation. The as-prepared core-shell nickel-iron-copper electrode is characterized with porous oxide shells and metallic cores. This tri-metal-based core-shell nickel-iron-copper electrode exhibits a remarkable activity toward water oxidation in alkaline medium with an overpotential of only 180 mV at a current density of 10 mA cm −2 . The core-shell NiFeCu electrode exhibits pH-dependent oxygen evolution reaction activity on the reversible hydrogen electrode scale, suggesting that non-concerted proton-electron transfers participate in catalyzing the oxygen evolution reaction. To the best of our knowledge, the as-fabricated core-shell nickel-iron-copper is one of the most promising oxygen evolution catalysts. Splitting water into high-energy fuel represents a renewable way to generate energy, yet the sluggish oxidation kinetics drives up technological costs. Here, the authors prepare tri-metallic core-shell electrodes using nickel, iron, and copper metals to accelerate electricity-driven water splitting.

Rational design of single atom catalyst is critical for efficient sustainable energy conversion. However, the atomic-level control of active sites is essential for electrocatalytic materials in alkaline electrolyte. Moreover, well-defined surface structures lead to in-depth understanding of catalytic mechanisms. Herein, we report a single-atomic-site ruthenium stabilized on defective nickel-iron layered double hydroxide nanosheets (Ru 1 /D-NiFe LDH). Under precise regulation of local coordination environments of catalytically active sites and the existence of the defects, Ru 1 /D-NiFe LDH delivers an ultralow overpotential of 18 mV at 10 mA cm −2 for hydrogen evolution reaction, surpassing the commercial Pt/C catalyst. Density functional theory calculations reveal that Ru 1 /D-NiFe LDH optimizes the adsorption energies of intermediates for hydrogen evolution reaction and promotes the O–O coupling at a Ru–O active site for oxygen evolution reaction. The Ru 1 /D-NiFe LDH as an ideal model reveals superior water splitting performance with potential for the development of promising water-alkali electrocatalysts. Rational design of single atom catalyst is critical for efficient sustainable energy conversion. Single-atomic-site ruthenium stabilized on defective nickel-iron layered double hydroxide nanosheets achieve superior HER and OER performance in alkaline media.

Accumulating evidence indicates that metabolism reprogramming is critically important to T cell differentiation, and manipulating metabolic pathways in T cells can shape their fate and function. During T cell differentiation, metabolism provides T cells with energy as well as precursors for various biological processes. Some key metabolic reactions, such as glycolysis, oxidative phosphorylation and fatty acid oxidation, are also considered to play important roles in T cell activation and differentiation. In this review, we will explain why cellular metabolism is important for the Th17/T-regulatory (Treg) cell balance and how metabolism reprogramming impacts this balance. Moreover, we will also discuss some important metabolic sensors, such as mammalian target of rapamycin, AMP-activated protein kinase, and some nuclear receptors. In addition, we will review specific small molecular compounds, which can shift the Th17/Treg cell balance and, therefore, have promising therapeutic roles. Finally, potential methods of manipulating Th17 cell metabolism for treating Th17-associated diseases will be discussed.

Domestic trade plays a key role in China’s rapid economic progress. However, the increased domestic trade causes significant variations in carbon emission transfer among provinces. This study adopted the multi-region input-output (MRIO) model and social network analysis (SNA) to estimate the carbon emission transfer. Furthermore, the carbon emission transfer network characteristics among 30 provinces and 27 sectors were analyzed by using interprovincial input-output tables for 2007, 2010, and 2012. The results showed that (1) Large differences exist in carbon emission transfer flow and its network characteristics between provinces. (2) The three industrial sectors of metal smelting and pressing sector, power, heat production, and supply sector, petroleum processing, coking, and nuclear fuel processing sector have high carbon emission transfer and pose a strong influence on the carbon emission transfer network. (3) Provinces of the eastern region have a “bidirectional spillover” role, while those of the western region have a mediating role as an “agent.” Provinces of the central region have a “main inflow” role. Finally, useful policy implications and suggestions of this study are summarized.

The electrooxidation of biomass platform molecules to produce highly value-added chemicals represents a promising technology for biomass utilization and carbon emission reduction. However, low production capacity and the lack of well-established engineering paradigms have constrained the practical application of this technology. Here, a green chemical process for the anion-exchange membrane (AEM) electrocatalytic 5-hydroxymethylfurfural oxidation (AEM-HMFOR) is proposed and applied to 2,5-furandicarboxylic acid (FDCA) production, with subsequent separation and purification. We demonstrate an optimized hundred-watt-scale AEM-HMFOR stack (164.8 W) for continuous FDCA production, with a high Faradaic efficiency (94.6%) and FDCA yield (96.2%) at 100% single-pass conversion efficiency (SPCE). This stack operates stably for over 100 hours with a space-time yield (STY) of 367.2 mg h −1 cm −2 . A membrane separation device is employed to purify FDCA with an overall purity of 99.8%. Techno-economic analysis (TEA) and life cycle assessment (LCA) have certified the economic viability and environmental sustainability of the proposed AEM-HMFOR technology. These findings represent a significant advancement in the practical application of large-scale AEM-HMFOR systems coupled to green H 2 production. Electrooxidation of biomass-derived molecules into value-added chemicals is promising but remains a challenge. Here, the authors report an integrated catalysis and purification process achieves stable synthesis of high-purity 2,5-furandicarboxylic acid in a hundred-watt-level electrolyzer.