Ruihu Lu

Renewably powered electrochemical CO₂ reduction (CO₂R) to alcohols presents a promising route to liquid fuels and chemicals. However, protonation of different intermediates often leads to mixed liquid and gas products, complicating separation and reducing economic feasibility. Here, we present a hydroxyl-affinity-tuning strategy that stabilizes hydroxyl-containing CO₂R intermediates away from interfacial water through constructing nano-metal interfaces, thereby favoring ethanol production. Theory-guided catalyst design directs nano-cobalt/Cu surfaces, delivering CO₂-to-ethanol Faradaic efficiencies (FE) of 62.17% and 45.32% under alkaline and acidic conditions, respectively, with ethanol partial current densities over ~300 mA cm^-2. In acidic media, the catalyst maintains ethanol production for 235 hours with an average FE of 44.74%. In situ spectroscopy and theoretical calculations reveal that nano-Co/Cu interfaces favor binding hydroxyl groups and thereby enriches C-OH species on the copper surface, redirects CO₂R pathways toward ethanol. This work provides a catalyst-centered strategy for designing interfacial architectures for selective alcohol synthesis. Future efforts should focus on translating this design principle into scalable systems for practical electrochemical CO₂ utilization.

Synergistic catalysis, where distinct active species collaboratively activate different substrates, provides a powerful strategy for achieving chemical transformations with enhanced efficiency. Although Al ₂ O ₃ and bulk aluminum species are widely employed as catalyst supports, they are seldom regarded as active centers, especially in hydrogenation. Here, we show that atomically dispersed Al species can catalyze acetylene conversion at elevated temperatures. Building on this insight, we have designed a synergistic catalyst featuring precisely controlled Al dual-atom sites paired with Ni nanoclusters, synthesized via a solid-transformation-coupled gas-adsorption strategy to overcome the typical activity-selectivity trade-off. Under mild, cost-effective conditions, this catalyst achieves nearly full acetylene conversion with ~90% ethylene selectivity and excellent long-term stability. In situ spectroscopy and theoretical calculations reveal a cooperative mechanism: Ni nanoclusters efficiently dissociate H ₂ into active hydrogen species (H*), while adjacent Al dual-atom sites shuttle the H* species to π-adsorbed acetylene, lowering the energy barrier for ethylene formation compared to over-hydrogenation and coke formation.

Dissolution of ruthenium (Ru) species under harsh anode operating conditions severely impedes the commercialization of non–iridium (Ir) proton exchange membrane water electrolyzers (PEMWEs). Here, we propose a catalyst design strategy that engineers phases beyond conventional atomic ordering, constructing a heterophase MoRuO _x catalyst (AC-MoRuO _x ). This catalyst achieves 10 milliamperes per square centimeter in an acidic oxygen evolution reaction with merely 180-millivolt overpotential while operating stably for >3000 hours. In PEMWE devices, AC-MoRuO _x delivers record durability at industrial current densities: ≥2000 hours at 1.0 ampere per square centimeter and 1000 hours at 1.5 amperes per square centimeter. We demonstrate that heterophase architecture and atomic arrangements reconfigure electronic structures and phase distribution, simultaneously optimizing active-site density and structural integrity. This breakthrough resolves the long-standing activity-stability trade-off in ruthenium-based catalysts.

CO₂/CO electrolysis offers a scalable pathway for electrosynthesis of multicarbon fuels and chemicals. However, current systems face challenges such as low energy and carbon efficiencies when operated at industrially relevant reaction rates. Our preliminary analysis revealed that the combination of high reaction rates and product crossover-induced pH reduction accelerates anode dissolution, leading to cathode poisoning and, ultimately, performance degradation. Here, we report a strategy to mitigate these challenges by dispersing a low concentration of nickel in an iridium oxide host to promote the stability of iridium species while inhibiting the oxidation of nickel sites. We synthesize a low-valence-nickel in iridium oxide anode material that exhibits high activity and stability for oxygen evolution, while remaining inactive for the oxidation of liquid products migrating from the cathode. In situ soft X-ray photoemission spectroscopy reveals the presence of active sites comprising Ni²⁺ and Ir⁴⁺ species. By incorporating this catalyst into an membrane electrode assembly setup, we achieve CO electroreduction on copper with a full-cell energy efficiency of 32% and a carbon efficiency of 73% at 1000 mA per square centimeter, alongside sustained stability over 1000 h of continuous operation.

Stable, nonprecious catalysts are vital for large-scale alkaline water electrolysis. Here, we report a grafted superstructure, MOF@POM, formed by self-assembling a metal-organic framework (MOF) with polyoxometalate (POM). In situ electrochemical transformation converts MOF into active metal (oxy)hydroxides to produce a catalyst with a low overpotential of 178 millivolts at 10 milliamperes per square centimeter in alkaline electrolyte. An anion exchange membrane water electrolyzer incorporating this catalyst achieves 3 amperes per square centimeter at 1.78 volts at 80°C and stable operation at 2 amperes per square centimeter for 5140 hours at room temperature. In situ electrochemical spectroscopy and theoretical studies reveal that the synergistic interactions between metal atoms create a fast electron-transfer channel from catalytic iron and cobalt sites, nickel, and tungsten in the polyoxometalate to the electrode, stabilizing the metal sites and preventing dissolution.

Precisely regulating the electron transfer capacity and Ru–O covalency of RuO₂-based catalysts is crucial and challenging for resolving the problem of the inadequate performance of RuO₂-based acidic oxygen evolution reaction (OER) catalysts in proton exchange membrane water electrolyzers (PEMWEs). Here, we propose to select Cr, an element with an atomic radius similar to that of Ru, for continuous doping of RuO₂ and to achieve continuous regulation of the electron transfer capacity and Ru–O covalency of RuO₂-based catalysts via adjusting the Cr content, thus optimizing the activity and stability of RuO₂-based catalysts. According to the experimental results, it was found that the acidic OER stability of Cr-doped RuO₂ catalysts (Cr_xRu_1−xO₂) tended to increase and then decrease with the gradual increase of the Cr doping level, and the tendency was almost consistent with the variation of the Ru–O covalency predicted by theoretical calculations. The RuO₂-based catalyst (Cr_0.31Ru_0.69O₂) showed optimal stability at a Cr/Ru ratio of 0.31/0.69 (Cr content similar to theoretical prediction), and was operated stably for over 1400 hours at a 10 mA cm⁻² current density with almost no degradation. Moreover, as the catalyst also has the best electron transfer ability, its activity is also the highest, requiring an overpotential of only 176 mV to deliver a 10 mA cm⁻² current density. Most importantly, the catalyst can be operated for at least 2300 hours at a 300 mA cm⁻² current density when applied to a PEMWE's anode, which strongly demonstrates its great potential for practical applications.

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.

Employing electrochemistry for the selective functionalization of liquid alkanes allows for sustainable and efficient production of high-value chemicals. However, the large potentials required for C(sp³)-H bond functionalization and low water solubility of such alkanes make it challenging. Here we discover that a Pt/IrO_x electrocatalyst with optimized Cl binding energy enables selective generation of Cl free radicals for C-H chlorination of alkanes. For instance, we achieve monochlorination of cyclohexane with a current up to 5 A, Faradaic efficiency (FE) up to 95% and stable performance over 100 h in aqueous KCl electrolyte. We further demonstrate that our system can directly utilize concentrated seawater derived from a solar evaporation reverse osmosis process, achieving a FE of 93.8% towards chlorocyclohexane at a current of 1 A. By coupling to a photovoltaic module, we showcase solar-driven production of chlorocyclohexane using concentrated seawater in a membrane electrode assembly cell without any external bias. Our findings constitute a sustainable pathway towards renewable energy driven chemicals manufacture using abundant feedstock at industrially relevant rates.

The electrochemical synthesis for value‐added chemicals and fuels via carbon dioxide reduction reaction (CO₂RR) offers an effective route to close the anthropogenic carbon cycle and store renewable energy. Currently, the copper‐based catalyst is still the only choice for generating various CO₂RR species beyond two electron products. However, the wide range of CO₂RR products generated on copper leads to low selectivity, and their low concentrations in electrolytes pose great costs in the downstream purification process and significantly challenge the scalability of this technology. To make this technology economically viable, enhancing product selectivity is crucial. In this review, we identify the primary CO₂RR species and discuss the latest insights into the reaction mechanisms controlling CO₂RR selectivity. Then, we examined factors that affect CO₂RR selectivity. Emphasizing these factors in catalyst design, we highlight the importance of advanced technologies to expand our knowledge and prospects for the future of the CO₂RR.